ALBERT

Description: Calibration of the passive cavity aerosol spectrometer probe for airborne determination of the size distribution Atmospheric Measurement Techniques, 6, 2349-2358, 2013 Author(s): Y. Cai, J. R. Snider, and P. Wechsler This work describes calibration methods for the particle sizing and particle concentration systems of the passive cavity aerosol spectrometer probe (PCASP). Laboratory calibrations conducted over six years, in support of the deployment of a PCASP on a cloud physics research aircraft, are analyzed. Instead of using the many calibration sizes recommended by the PCASP manufacturer, a relationship between particle diameter and scattered light intensity is established using three sizes of mobility-selected polystyrene latex particles, one for each amplifier gain stage. In addition, studies of two factors influencing the PCASP's determination of the particle size distribution – amplifier baseline and particle shape – are conducted. It is shown that the PCASP-derived size distribution is sensitive to adjustments of the sizing system's baseline voltage, and that for aggregates of spheres, a PCASP-derived particle size and a sphere-equivalent particle size agree within uncertainty dictated by the PCASP's sizing resolution. Robust determinations of aerosol concentration, and size distribution, also require calibration of the PCASP's aerosol flowrate sensor. Sensor calibrations, calibration drift, and the sensor's non-linear response are documented.

Description: Experimental quantification of contact freezing in an electrodynamic balance Atmospheric Measurement Techniques, 6, 2373-2382, 2013 Author(s): N. Hoffmann, A. Kiselev, D. Rzesanke, D. Duft, and T. Leisner Heterogeneous nucleation of ice in a supercooled water droplet induced by external contact with a dry aerosol particle has long been known to be more effective than freezing induced by the same nucleus immersed in the droplet. However, the experimental quantification of contact freezing is challenging. Here we report an experimental method to determine the temperature-dependent ice nucleation probability of size-selected aerosol particles. The method is based on the suspension of supercooled charged water droplets in a laminar flow of air containing aerosol particles as contact freezing nuclei. The rate of droplet–particle collisions is calculated numerically with account for Coulomb attraction, drag force and induced dipole interaction between charged droplet and aerosol particles. The calculation is verified by direct counting of aerosol particles collected by a levitated droplet. By repeating the experiment on individual droplets for a sufficient number of times, we are able to reproduce the statistical freezing behavior of a large ensemble of supercooled droplets and measure the average rate of freezing events. The freezing rate is equal to the product of the droplet–particle collision rate and the probability of freezing on a single contact, the latter being a function of temperature, size and composition of the contact ice nuclei. Based on these observations, we show that for the types of particles investigated so far, contact freezing is the dominating freezing mechanism on the timescale of our experiment.

Description: Similarity estimators for irregular and age uncertain time series Climate of the Past Discussions, 9, 5299-5346, 2013 Author(s): K. Rehfeld and J. Kurths Paleoclimate time series are often irregularly sampled and age uncertain, which is an important technical challenge to overcome for successful reconstruction of past climate variability and dynamics. Visual comparison and interpolation-based linear correlation approaches have been used to infer dependencies from such proxy time series. While the first is subjective, not measurable and not suitable for the comparison of many datasets at a time, the latter introduces interpolation bias, and both face difficulties if the underlying dependencies are nonlinear. In this paper we investigate similarity estimators that could be suitable for the quantitative investigation of dependencies in irregular and age uncertain time series. We compare the Gaussian-kernel based cross correlation (gXCF, Rehfeld et al., 2011) and mutual information (gMI, Rehfeld et al., 2013) against their interpolation-based counterparts and the new event synchronization function (ESF). We test the efficiency of the methods in estimating coupling strength and coupling lag numerically, using ensembles of synthetic stalagmites with short, autocorrelated, linear and nonlinearly coupled proxy time series, and in the application to real stalagmite time series. In the linear test case coupling strength increases are identified consistently for all estimators, while in the nonlinear test case the correlation-based approaches fail. The lag at which the time series are coupled is identified correctly as the maximum of the similarity functions in around 60–55% (in the linear case) to 53–42% (for the nonlinear processes) of the cases when the dating of the synthetic stalagmite is perfectly precise. If the age uncertainty increases beyond 5% of the time series length, however, the true coupling lag is not identified more often than the others for which the similarity function was estimated. Age uncertainty contributes up to half of the uncertainty in the similarity estimation process. Time series irregularity contributes less, particularly for the adapted Gaussian-kernel based estimators and the event synchronization function. The introduced link strength concept summarizes the hypothesis test results and balances the individual strengths of the estimators: while gXCF is particularly suitable for short and irregular time series, gMI and the ESF can identify nonlinear dependencies. ESF could, in particular, be suitable to study extreme event dynamics in paleoclimate records. Programs to analyze paleoclimatic time series for significant dependencies are included in a freely available software toolbox.

Description: Impact of precession on the climate, vegetation and fire activity in southern Africa during MIS4 Climate of the Past Discussions, 9, 5391-5438, 2013 Author(s): M.-N. Woillez, G. Levavasseur, A.-L. Daniau, M. Kageyama, D. H. Urrego, and M.-F. Sánchez-Goñi The relationships between climate, vegetation and fires are a major subject of investigation in the context of climate change. In southern Africa, fire is known to play a crucial role in the existence of grasslands and Mediterranean-like biomes. Microcharcoal-based reconstructions of past fire activity in that region have shown a tight correlation between grass-fueled fires and the precessional cycle, with maximum fire activity during maxima of the climatic precession index. These changes have been interpreted as the result of changes in fuel load in response to precipitation changes in eastern southern Africa. Here we use the general circulation model IPSL_CM5A and the dynamical vegetation model LPJ-LMfire to investigate the response of climate, vegetation and fire activity to precession changes in southern Africa during Marine Isotopic Stage 4. We perform two climatic simulations, for a maximum and minimum of the precession index, and use a statistical downscaling method to increase the spatial resolution of the IPSL_CM5A outputs over southern Africa and perform high-resolution simulations of the vegetation and fire activity. Our results show an anti-correlation between the North and South African monsoons in response to precession changes. A decrease of the precession climatic index leads to a precipitation decrease in the summer rainfall area of southern Africa. The drying of climate leads to a decrease of vegetation cover and fire activity. Our results are in qualitative agreement with data and confirm that fire activity in southern Africa is strongly dependent on the vegetation type.

Description: Validation and empirical correction of MODIS AOT and AE over ocean Atmospheric Measurement Techniques, 6, 2455-2475, 2013 Author(s): N. A. J. Schutgens, M. Nakata, and T. Nakajima We present a validation study of Collection 5 MODIS level 2 Aqua and Terra AOT (aerosol optical thickness) and AE (Ångström exponent) over ocean by comparison to coastal and island AERONET (AErosol RObotic NETwork) sites for the years 2003–2009. We show that MODIS (MODerate-resolution Imaging Spectroradiometer) AOT exhibits significant biases due to wind speed and cloudiness of the observed scene, while MODIS AE, although overall unbiased, exhibits less spatial contrast on global scales than the AERONET observations. The same behaviour can be seen when MODIS AOT is compared against Maritime Aerosol Network (MAN) data, suggesting that the spatial coverage of our datasets does not preclude global conclusions. Thus, we develop empirical correction formulae for MODIS AOT and AE that significantly improve agreement of MODIS and AERONET observations. We show these correction formulae to be robust. Finally, we study random errors in the corrected MODIS AOT and AE and show that they mainly depend on AOT itself, although small contributions are present due to wind speed and cloud fraction in AOT random errors and due to AE and cloud fraction in AE random errors. Our analysis yields significantly higher random AOT errors than the official MODIS error estimate (0.03 + 0.05 τ), while random AE errors are smaller than might be expected. This new dataset of bias-corrected MODIS AOT and AE over ocean is intended for aerosol model validation and assimilation studies, but also has consequences as a stand-alone observational product. For instance, the corrected dataset suggests that much less fine mode aerosol is transported across the Pacific and Atlantic oceans.

Description: Ensemble meteorological reconstruction using circulation analogues of 1781–1785 Climate of the Past Discussions, 9, 5157-5182, 2013 Author(s): P. Yiou, M. Boichu, R. Vautard, M. Vrac, S. Jourdain, E. Garnier, F. Fluteau, and L. Menut This paper uses a method of atmospheric flow analogues to reconstruct an ensemble of atmospheric variables (namely sea-level pressure, surface temperature and wind speed) between 1781 and 1785. The properties of this ensemble are investigated and tested against observations of temperature. The goal of the paper is to assess whether the atmospheric circulation during the Laki volcanic eruption (in 1783) and the subsequent winter were similar to the conditions that prevailed in the winter 2009/2010 and during spring 2010. We find that the three months following the Laki eruption in June 1783 barely have analogues in 2010. The cold winter of 1783/1784 yields circulation analogues in 2009/2010. Our analysis suggests that it is unlikely that the Laki eruption was responsible for the cold winter of 1783/1784, of the relatively short memory of the atmospheric circulation.

Description: Seasonal changes in glacial polynya activity inferred from Weddell Sea varves Climate of the Past Discussions, 9, 5123-5156, 2013 Author(s): D. Sprenk, M. E. Weber, G. Kuhn, V. Wennrich, T. Hartmann, and K. Seelos The Weddell Sea and the associated Filchner-Rønne Ice Shelf constitute key regions for global bottom-water production today. However, little is known about bottom-water production under different climate and ice-sheet conditions. Therefore, we studied core PS1795, which consists primarily of fine-grained siliciclastic varves that were deposited on contourite ridges in the southeastern Weddell Sea during the Last Glacial Maximum (LGM). We conducted high-resolution X-ray fluorescence (XRF) analysis and grain-size measurements with the RADIUS tool (Seelos and Sirocko, 2005) using thin sections to characterize the two seasonal components of the varves at sub-mm resolution to distinguish the seasonal components of the varves. Bright layers contain coarser grains that can mainly be identified as quartz in the medium to coarse silt grain size. They also contain higher amounts of Si, Zr, Ca, and Sr, as well as more ice-rafted debris (IRD). Dark layers, on the other hand, contain finer particles such as mica and clay minerals from the chlorite and illite groups. In addition, chemical elements, Fe, Ti, Rb, and K are elevated as well. Based on these findings as well as on previous analyses on neighbouring cores, we propose a model of glacially enhanced thermohaline convection in front of a grounded ice sheet that is supported by seasonally variable coastal polynya activity. Accordingly, katabatic (i.e. offshore blowing) winds removed sea ice from the ice edge, leading to coastal polynya formation. We suggest that glacial processes were similar to today with stronger katabatic winds and enhanced coastal polynya activity during the winter season. If this is correct, silty layers are likely glacial winter deposits, when brine rejection was increased, leading to enhanced bottom water formation and increased sediment transport. Vice versa, finer-grained clayey layers were then deposited during summer, when coastal polynya activity was likely reduced.

Description: A neural network algorithm for cloud fraction estimation using NASA-Aura OMI VIS radiance measurements Atmospheric Measurement Techniques, 6, 2301-2309, 2013 Author(s): G. Saponaro, P. Kolmonen, J. Karhunen, J. Tamminen, and G. de Leeuw The discrimination of cloudy from cloud-free pixels is required in almost any estimate of a parameter retrieved from satellite data in the ultraviolet (UV), visible (VIS) or infrared (IR) parts of the electromagnetic spectrum. In this paper we report on the development of a neural network (NN) algorithm to estimate cloud fractions using radiances measured at the top of the atmosphere with the NASA-Aura Ozone Monitoring Instrument (OMI). We present and discuss the results obtained from the application of two different types of neural networks, i.e., extreme learning machine (ELM) and back propagation (BP). The NNs were trained with an OMI data sets existing of six orbits, tested with three other orbits and validated with another two orbits. The results were evaluated by comparison with cloud fractions available from the MODerate Resolution Imaging Spectrometer (MODIS) flying on Aqua in the same constellation as OMI, i.e., with minimal time difference between the OMI and MODIS observations. The results from the ELM and BP NNs are compared. They both deliver cloud fraction estimates in a fast and automated way, and they both performs generally well in the validation. However, over highly reflective surfaces, such as desert, or in the presence of dust layers in the atmosphere, the cloud fractions are not well predicted by the neural network. Over ocean the two NNs work equally well, but over land ELM performs better.

Description: Validation of stratospheric and mesospheric ozone observed by SMILES from International Space Station Atmospheric Measurement Techniques, 6, 2311-2338, 2013 Author(s): Y. Kasai, H. Sagawa, D. Kreyling, E. Dupuy, P. Baron, J. Mendrok, K. Suzuki, T. O. Sato, T. Nishibori, S. Mizobuchi, K. Kikuchi, T. Manabe, H. Ozeki, T. Sugita, M. Fujiwara, Y. Irimajiri, K. A. Walker, P. F. Bernath, C. Boone, G. Stiller, T. von Clarmann, J. Orphal, J. Urban, D. Murtagh, E. J. Llewellyn, D. Degenstein, A. E. Bourassa, N. D. Lloyd, L. Froidevaux, M. Birk, G. Wagner, F. Schreier, J. Xu, P. Vogt, T. Trautmann, and M. Yasui We observed ozone (O 3 ) in the vertical region between 250 and 0.0005 hPa (~ 12–96 km) using the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the Japanese Experiment Module (JEM) of the International Space Station (ISS) between 12 October 2009 and 21 April 2010. The new 4 K superconducting heterodyne receiver technology of SMILES allowed us to obtain a one order of magnitude better signal-to-noise ratio for the O 3 line observation compared to past spaceborne microwave instruments. The non-sun-synchronous orbit of the ISS allowed us to observe O 3 at various local times. We assessed the quality of the vertical profiles of O 3 in the 100–0.001 hPa (~ 16–90 km) region for the SMILES NICT Level 2 product version 2.1.5. The evaluation is based on four components: error analysis; internal comparisons of observations targeting three different instrumental setups for the same O 3 625.371 GHz transition; internal comparisons of two different retrieval algorithms; and external comparisons for various local times with ozonesonde, satellite and balloon observations (ENVISAT/MIPAS, SCISAT/ACE-FTS, Odin/OSIRIS, Odin/SMR, Aura/MLS, TELIS). SMILES O 3 data have an estimated absolute accuracy of better than 0.3 ppmv (3%) with a vertical resolution of 3–4 km over the 60 to 8 hPa range. The random error for a single measurement is better than the estimated systematic error, being less than 1, 2, and 7%, in the 40–1, 80–0.1, and 100–0.004 hPa pressure regions, respectively. SMILES O 3 abundance was 10–20% lower than all other satellite measurements at 8–0.1 hPa due to an error arising from uncertainties of the tangent point information and the gain calibration for the intensity of the spectrum. SMILES O 3 from observation frequency Band-B had better accuracy than that from Band-A. A two month period is required to accumulate measurements covering 24 h in local time of O 3 profile. However such a dataset can also contain variation due to dynamical, seasonal, and latitudinal effects.

Description: Is blue intensity ready to replace maximum latewood density as a strong temperature proxy? A tree-ring case study on Scots pine from northern Sweden Climate of the Past Discussions, 9, 5227-5261, 2013 Author(s): J. A. Björklund, B. E. Gunnarson, K. Seftigen, J. Esper, and H. W. Linderholm At high latitudes, where low temperatures mainly limit tree-growth, measurements of wood density (e.g. Maximum Latewood Density, MXD) using the X-Ray methodology provide a temperature proxy that is superior to that of TRW. Density measurements are however costly and time consuming and have lead to experimentation with optical flatbed scanners to produce Maximum Blue Intensity (BI max ). BI max is an excellent proxy for density on annual scale but very limited in skill on centennial scale. Discolouration between samples is limiting BI max where specific brightnesses can have different densities. To overcome this, the new un-exploited parameter Δ blue intensity (ΔBI) was constructed by using the brightness in the earlywood (BI EW ) as background, (BI max − BI EW = ΔBI). This parameter was tested on X-Ray material (MXD − earlywood density = ΔMXD) and showed great potential both as a quality control and as a booster of climate signals. Unfortunately since the relationship between grey scale and density is not linear, and between-sample brightness can differ tremendously for similar densities, ΔBI cannot fully match ΔMXD in skill as climate proxy on centennial scale. For ΔBI to stand alone, the range of brightness/density offset must be reduced. Further studies are needed to evaluate this possibility, and solutions might include heavier sample treatment (reflux with chemicals) or image-data treatment (digitally manipulating base-line levels of brightness).

Description: The Atmospheric radiation measurement (ARM) program network of microwave radiometers: instrumentation, data, and retrievals Atmospheric Measurement Techniques, 6, 2359-2372, 2013 Author(s): M. P. Cadeddu, J. C. Liljegren, and D. D. Turner The Climate Research Facility of the US Department of Energy's Atmospheric Radiation Measurement (ARM) Program operates a network of ground-based microwave radiometers. Data and retrievals from these instruments have been available to the scientific community for almost 20 yr. In the past five years the network has expanded to include a total of 22 microwave radiometers deployed in various locations around the world. The new instruments cover a frequency range between 22 and 197 GHz and are consistently and automatically calibrated. The latest addition to the network is a new generation of three-channel radiometers, currently in the early stage of deployment at all ARM sites. The network has been specifically designed to achieve increased accuracy in the retrieval of precipitable water vapor (PWV) and cloud liquid water path (LWP) with the long-term goal of providing the scientific community with reliable, calibrated radiometric data and retrievals of important geophysical quantities with well-characterized uncertainties. The radiometers provide high-quality, continuous datasets that can be utilized in a wealth of applications and scientific studies. This paper presents an overview of the microwave instrumentation, calibration procedures, data, and retrievals that are available for download from the ARM data archive.

Description: Airborne sun photometer PLASMA: concept, measurements, comparison of aerosol extinction vertical profile with lidar Atmospheric Measurement Techniques, 6, 2383-2389, 2013 Author(s): Y. Karol, D. Tanré, P. Goloub, C. Vervaerde, J. Y. Balois, L. Blarel, T. Podvin, A. Mortier, and A. Chaikovsky A 15-channel airborne sun-tracking photometer has been developed. The instrument provides aerosol optical depths over a wide spectral range (0.34–2.25 μm) with an accuracy (ΔAOD) of approximately 0.01. Taking measurements at different altitudes allow us to derive the aerosol extinction vertical profile. Thanks to the wide spectral range of the instrument, information on the aerosol size distribution along the vertical is also available.

Description: McClear: a new model estimating downwelling solar radiation at ground level in clear-sky conditions Atmospheric Measurement Techniques, 6, 2403-2418, 2013 Author(s): M. Lefèvre, A. Oumbe, P. Blanc, B. Espinar, B. Gschwind, Z. Qu, L. Wald, M. Schroedter-Homscheidt, C. Hoyer-Klick, A. Arola, A. Benedetti, J. W. Kaiser, and J.-J. Morcrette A new fast clear-sky model called McClear was developed to estimate the downwelling shortwave direct and global irradiances received at ground level under clear skies. It is a fully physical model replacing empirical relations or simpler models used before. It exploits the recent results on aerosol properties, and total column content in water vapour and ozone produced by the MACC project (Monitoring Atmosphere Composition and Climate). It accurately reproduces the irradiance computed by the libRadtran reference radiative transfer model with a computational speed approximately 10 5 times greater by adopting the abaci, or look-up table, approach combined with interpolation functions. It is therefore suited for geostationary satellite retrievals or numerical weather prediction schemes with many pixels or grid points, respectively. McClear irradiances were compared to 1 min measurements made in clear-sky conditions at several stations within the Baseline Surface Radiation Network in various climates. The bias for global irradiance comprises between −6 and 25 W m −2 . The RMSE ranges from 20 W m −2 (3% of the mean observed irradiance) to 36 W m −2 (5%) and the correlation coefficient ranges between 0.95 and 0.99. The bias for the direct irradiance comprises between −48 and +33 W m −2 . The root mean square error (RMSE) ranges from 33 W m −2 (5%) to 64 W m −2 (10%). The correlation coefficient ranges between 0.84 and 0.98. This work demonstrates the quality of the McClear model combined with MACC products, and indirectly the quality of the aerosol properties modelled by the MACC reanalysis.

Description: Ten years of MIPAS measurements with ESA Level 2 processor V6 – Part 1: Retrieval algorithm and diagnostics of the products Atmospheric Measurement Techniques, 6, 2419-2439, 2013 Author(s): P. Raspollini, B. Carli, M. Carlotti, S. Ceccherini, A. Dehn, B. M. Dinelli, A. Dudhia, J.-M. Flaud, M. López-Puertas, F. Niro, J. J. Remedios, M. Ridolfi, H. Sembhi, L. Sgheri, and T. von Clarmann The MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) instrument on the Envisat (Environmental satellite) satellite has provided vertical profiles of the atmospheric composition on a global scale for almost ten years. The MIPAS mission is divided in two phases: the full resolution phase, from 2002 to 2004, and the optimized resolution phase, from 2005 to 2012, which is characterized by a finer vertical and horizontal sampling attained through a reduction of the spectral resolution. While the description and characterization of the products of the ESA processor for the full resolution phase has been already described in previous papers, in this paper we focus on the performances of the latest version of the ESA (European Space Agency) processor, named ML2PP V6 (MIPAS Level 2 Prototype Processor), which has been used for reprocessing the entire mission. The ESA processor had to perform the operational near real time analysis of the observations and its products needed to be available for data assimilation. Therefore, it has been designed for fast, continuous and automated analysis of observations made in quite different atmospheric conditions and for a minimum use of external constraints in order to avoid biases in the products. The dense vertical sampling of the measurements adopted in the second phase of the MIPAS mission resulted in sampling intervals finer than the instantaneous field of view of the instrument. Together with the choice of a retrieval grid aligned with the vertical sampling of the measurements, this made ill-conditioned the retrieval problem of the MIPAS operational processor. This problem has been handled with minimal changes to the original retrieval approach but with significant improvements nonetheless. The Levenberg–Marquardt method, already present in the retrieval scheme for its capability to provide fast convergence for nonlinear problems, is now also exploited for the reduction of the ill-conditioning of the inversion. An expression specifically designed for the regularizing Levenberg–Marquardt method has been implemented for the computation of the covariance matrices and averaging kernels of the retrieved products. The regularization of the Levenberg–Marquardt method is controlled by the convergence criteria and is deliberately kept weak. The resulting oscillations of the retrieved profile are a posteriori damped by an innovative self-adapting Tikhonov regularization. The convergence criteria and the weakness of the self-adapting regularization ensure that minimum constraints are used and the best vertical resolution obtainable from the measurements is achieved in all atmospheric conditions. Random and systematic errors, as well as vertical and horizontal resolution are compared in the two phases of the mission for all products, namely: temperature, H 2O , O 3 , HNO 3 , CH 4 , N 2O , NO 2 , CFC-11, CFC-12, N 2 O 5 and ClONO 2 . The use in the two phases of the mission of different optimized sets of spectral intervals ensures that, despite the different spectral resolutions, comparable performances are obtained in the whole MIPAS mission in terms of random and systematic errors, while the vertical resolution and the horizontal resolution are significantly better in the case of the optimized resolution measurements.

Description: Ground-based stratospheric O 3 and HNO 3 measurements at Thule, Greenland: an intercomparison with Aura MLS observations Atmospheric Measurement Techniques, 6, 2441-2453, 2013 Author(s): I. Fiorucci, G. Muscari, L. Froidevaux, and M. L. Santee In response to the need for improving our understanding of the evolution and the interannual variability of the winter Arctic stratosphere, in January 2009 a Ground-Based Millimeter-wave Spectrometer (GBMS) was installed at the Network for the Detection of Atmospheric Composition Change (NDACC) site in Thule (76.5° N, 68.8° W), Greenland. In this work, stratospheric GBMS O 3 and HNO 3 vertical profiles obtained from Thule during the winters 2010 (HNO 3 only), 2011 and 2012 are characterized and intercompared with co-located measurements of the Aura Microwave Limb Sounder (MLS) experiment. Using a recently developed algorithm based on Optimal Estimation, we find that the GBMS O 3 retrievals show good sensitivity (〉 80%) to atmospheric variations between ~ 17 and ~ 50 km, where their 1σ uncertainty is estimated to be the larger of ~ 11% or 0.2 ppmv. Similarly, HNO 3 profiles can be considered for scientific use between ~ 17 and ~ 45 km altitude, with a 1σ uncertainty that amounts to the larger of 15% or 0.2 ppbv. Comparisons with Aura MLS version 3.3 observations show that, on average, GBMS O 3 mixing ratios are biased negatively with respect to MLS throughout the stratosphere, with differences ranging between ~ 0.3 ppmv (8%) and 0.9 ppmv (18%) in the 17–50 km vertical range. GBMS HNO 3 values display instead a positive bias with respect to MLS up to 26 km, reaching a maximum of ~ 1 ppbv (10%) near the mixing ratio profile peak. O 3 and HNO 3 values from the two datasets prove to be well correlated at all altitudes, although their correlations worsen at the lower end of the altitude ranges considered. Column contents of GBMS and MLS O 3 (from 20 km upwards) and HNO 3 (from 17 km upwards) correlate very well and indicate that GBMS measurements can provide valuable estimates of column interannual and seasonal variations for these compounds.

Description: Inter-calibration of polar imager solar channels using SEVIRI Atmospheric Measurement Techniques, 6, 2495-2508, 2013 Author(s): J. F. Meirink, R. A. Roebeling, and P. Stammes Accurate calibration of satellite imagers is a prerequisite for using their measurements in climate applications. Here we present a method for the inter-calibration of geostationary and polar-orbiting imager solar channels based on regressions of collocated near-nadir reflectances. Specific attention is paid to correcting for differences in spectral response between instruments. The method is used to calibrate the solar channels of the Spinning Enhanced Visible and Infrared Imager (SEVIRI) on the geostationary Meteosat satellite with corresponding channels of the Moderate Resolution Imaging Spectroradiometer (MODIS) on the polar-orbiting Aqua satellite. The SEVIRI operational calibration is found to be stable during the years 2004 to 2009, but offset by −8, −6, and +3.5 % for channels 1 (0.6 μm), 2 (0.8 μm), and 3 (1.6 μm), respectively. These results are robust for a range of choices that can be made regarding data collocation and selection, as long as the viewing and illumination geometries of the two instruments are matched. Uncertainties in the inter-calibration method are estimated to be 1 % for channel 1 and 1.5 % for channels 2 and 3. A specific application of our method is the inter-calibration of polar imagers using SEVIRI as a transfer instrument. This offers an alternative to direct inter-calibration, which in general has to rely on high-latitude collocations. Using this method we have tied MODIS-Terra and Advanced Very High Resolution Radiometer (AVHRR) instruments on National Oceanic and Atmospheric Administration (NOAA) satellites 17 and 18 to MODIS-Aqua for the years 2007 to 2009. While reflectances of the two MODIS instruments differ less than 2 % for all channels considered, deviations of an existing AVHRR calibration from MODIS-Aqua reach −3.5 and +2.5 % for the 0.8 and 1.6 μm channels, respectively.

Description: Using ocean-glint scattered sunlight as a diagnostic tool for satellite remote sensing of greenhouse gases Atmospheric Measurement Techniques, 6, 2509-2520, 2013 Author(s): A. Butz, S. Guerlet, O. P. Hasekamp, A. Kuze, and H. Suto Spectroscopic measurements of sunlight backscattered by the Earth's surface is a technique widely used for remote sensing of atmospheric constituent concentrations from space. Thereby, remote sensing of greenhouse gases poses particularly challenging accuracy requirements for instrumentation and retrieval algorithms which, in general, suffer from various error sources. Here, we investigate a method that helps disentangle sources of error for observations of sunlight backscattered from the glint spot on the ocean surface. The method exploits the backscattering characteristics of the ocean surface, which is bright for glint geometry but dark for off-glint angles. This property allows for identifying a set of clean scenes where light scattering due to particles in the atmosphere is negligible such that uncertain knowledge of the lightpath can be excluded as a source of error. We apply the method to more than 3 yr of ocean-glint measurements by the Thermal And Near infrared Sensor for carbon Observation (TANSO) Fourier Transform Spectrometer (FTS) onboard the Greenhouse Gases Observing Satellite (GOSAT), which aims at measuring carbon dioxide (CO 2 ) and methane (CH 4 ) concentrations. The proposed method is able to clearly monitor recent improvements in the instrument calibration of the oxygen (O 2 ) A-band channel and suggests some residual uncertainty in our knowledge about the instrument. We further assess the consistency of CO 2 retrievals from several absorption bands between 6400 cm −1 (1565 nm) and 4800 cm −1 (2100 nm) and find that the absorption bands commonly used for monitoring of CO 2 dry air mole fractions from GOSAT allow for consistency better than 1.5 ppm. Usage of other bands reveals significant inconsistency among retrieved CO 2 concentrations pointing at inconsistency of spectroscopic parameters.

Description: Migrating subtropical front and Agulhas Return Current affect the southwestern Indian Ocean during the late Quaternary Climate of the Past Discussions, 9, 5521-5551, 2013 Author(s): D. K. Naik, R. Saraswat, N. Khare, A. C. Pandey, and R. Nigam The position of sub-tropical front (STF), Agulhas Current (AC) and Agulhas Return Current (ARC) controls the hydrography of southwestern Indian Ocean. Although, equator-ward migration of STF and reduction in Agulhas leakage has been reported during the last glacial period, the fate of ARC during the last glacial–interglacial cycle is not clear. Therefore, in order to understand changes in the position and strength of ARC during the last glacial–interglacial cycle, here we reconstruct hydrographic changes in the southwestern Indian Ocean from temporal variation in planktic foraminiferal abundance, stable isotopic ratio (δ 18 O) and trace metal ratio (Mg / Ca) of planktic foraminifera Globigerina bulloides in a core collected from the Agulhas Retroflection Region (ARR) in the southwestern Indian Ocean. Increased abundance of G. bulloides suggests that the productivity in the southwestern Indian Ocean increased during glacial period which confirms previous reports of high glacial productivity in the Southern Ocean. The increased productivity was likely driven by a combination of equator-ward migration of subtropical front and westerlies. Increase in relative abundance of Neogloboquadrina pachyderma Dextral suggests warming of ARR leading to strong thermocline in the southwestern Indian Ocean during the last glacial period. We suggest that the warming of Agulhas Retroflection Region was driven by strengthened ARC which shifted to the east of its present location, thus bringing warmer and saltier water to the southwestern Indian Ocean. Therefore, it is inferred that over the last glacial–interglacial cycle, the hydrography of southwestern Indian Ocean was driven by an eastward shift of retroflection region as well as migrating subtropical front.

Description: The response of the Peruvian Upwelling Ecosystem to centennial-scale global change during the last two millennia Climate of the Past Discussions, 9, 5479-5519, 2013 Author(s): R. Salvatteci, D. Gutiérrez, D. Field, A. Sifeddine, L. Ortlieb, I. Bouloubassi, M. Boussafir, H. Boucher, and F. Cetin The Tropical Pacific ocean-atmosphere system influences global climate on interannual, decadal, as well as at longer timescales. Given the uncertainties in the response of the Tropical Pacific to the ongoing greenhouse effect, it is important to assess the natural range of the Tropical Pacific climate variability in response to global natural changes, and to understand the underlying mechanisms. The Peruvian Upwelling Ecosystem (PUE) represents an ideal area to reconstruct past changes in ocean-atmosphere systems because productivity and subsurface oxygenation are strongly linked to changes in the strength of the Walker circulation. Throughout the last 2000 yr, warmer (the Roman Warm Period [RWP], the Medieval Climate Anomaly [MCA] and the Current Warm Period [CWP]), and colder (the Dark Ages Cold Period [DACP] and Little Ice Age [LIA]) intervals occurred with considerable changes around the globe. In order to reconstruct the PUE response to these climatic periods and reveal the underlying mechanisms, we use a multi-proxy approach including organic and inorganic proxies in finely laminated sediments retrieved off Pisco (~ 14° S), Peru. Our results indicate that the PUE exhibited a La Niña-like mean state during the warm periods, characterized by an intense OMZ and high marine productivity. During cold periods the PUE exhibited an El Niño-like mean state, characterized by a weak OMZ and low marine productivity. Comparing our results with other relevant paleoclimatic reconstructions revealed that changes in the strength of the Walker circulation and the expansion/contraction of the South Pacific Sub-tropical High controlled productivity and subsurface oxygenation in the PUE during the last two millennia. This indicate that large scale circulation changes are the driving forces in maintaining productivity and subsurface oxygenation off Peru at centennial time scales during the past two millennia.

Description: Cumulated insolation: a simple explanation of Milankovitch's forcing on climate changes Climate of the Past Discussions, 9, 5553-5568, 2013 Author(s): F. Marra The occurrence of the sudden melting of the ice sheets during the glacial terminations is explained in this paper as the consequence of the combined role of the minima and the maxima of mean summer insolation on the Northern Hemisphere, providing a new contribution to understand the mechanisms ruling glacial forcing. Indeed, no satisfactory answer has been provided so far to the question why one specific maximum, after a series of consecutive maxima of insolation, has the potentiality to trigger a deglaciation. The explanation proposed in this paper accounts for a pre-conditioning factor, represented by "mild" (warmer) minimum, followed by a sufficiently warm maximum as the conditions that cause the end of a glacial cycle. These conditions are realized whenever the sum of the values of each consecutive minima and maxima ("cumulated insolation") on the curve of mean summer insolation at 65° N exceeds 742 Watt m −2 . The comparison of the succession of these cumulated insolation values with the astronomically tuned Oxygen isotopes record provides a satisfactory match with the occurrence of all the glacial terminations in the last 800 ka.

Description: Parameterizing radiative transfer to convert MAX-DOAS dSCDs into near-surface box-averaged mixing ratios Atmospheric Measurement Techniques, 6, 1521-1532, 2013 Author(s): R. Sinreich, A. Merten, L. Molina, and R. Volkamer We present a novel parameterization method to convert multi-axis differential optical absorption spectroscopy (MAX-DOAS) differential slant column densities (dSCDs) into near-surface box-averaged volume mixing ratios. The approach is applicable inside the planetary boundary layer under conditions with significant aerosol load, and builds on the increased sensitivity of MAX-DOAS near the instrument altitude. It parameterizes radiative transfer model calculations and significantly reduces the computational effort, while retrieving ~ 1 degree of freedom. The biggest benefit of this method is that the retrieval of an aerosol profile, which usually is necessary for deriving a trace gas concentration from MAX-DOAS dSCDs, is not needed. The method is applied to NO 2 MAX-DOAS dSCDs recorded during the Mexico City Metropolitan Area 2006 (MCMA-2006) measurement campaign. The retrieved volume mixing ratios of two elevation angles (1° and 3°) are compared to volume mixing ratios measured by two long-path (LP)-DOAS instruments located at the same site. Measurements are found to agree well during times when vertical mixing is expected to be strong. However, inhomogeneities in the air mass above Mexico City can be detected by exploiting the different horizontal and vertical dimensions probed by the MAX-DOAS and LP-DOAS instruments. In particular, a vertical gradient in NO 2 close to the ground can be observed in the afternoon, and is attributed to reduced mixing coupled with near-surface emission inside street canyons. The existence of a vertical gradient in the lower 250 m during parts of the day shows the general challenge of sampling the boundary layer in a representative way, and emphasizes the need of vertically resolved measurements.

Description: Polarization data from SCIAMACHY limb backscatter observations compared to vector radiative transfer model simulations Atmospheric Measurement Techniques, 6, 1503-1520, 2013 Author(s): P. Liebing, K. Bramstedt, S. Noël, V. Rozanov, H. Bovensmann, and J. P. Burrows SCIAMACHY is a passive imaging spectrometer onboard ENVISAT designed to obtain trace gas abundances from measured radiances and irradiances in the UV to SWIR range in nadir-, limb- and occultation-viewing modes. Its grating spectrometer introduces a substantial sensitivity to the polarization of the incoming light with nonnegligible effects on the radiometric calibration. To be able to correct for the polarization sensitivity, SCIAMACHY utilizes broadband Polarization Measurement Devices (PMDs). While for the nadir-viewing mode the measured atmospheric polarization has been validated against POLDER data (Tilstra and Stammes, 2007, 2010), a similar validation study regarding the limb-viewing mode has not yet been performed. This paper aims at an assessment of the quality of the SCIAMACHY limb polarization data. Since limb polarization measurements by other air/spaceborne instruments in the spectral range of SCIAMACHY are not available, a comparison with radiative transfer simulations by SCIATRAN V3.1 (Rozanov et al., 2013) using a wide range of atmospheric parameters is performed. SCIATRAN is a vector radiative transfer model (VRTM) capable of performing calculations of the multiply scattered radiance in a spherically symmetric atmosphere. The study shows that the limb polarization data exhibit a large time-dependent bias that decreases with wavelength. Possible reasons for this bias are a still unknown combination of insufficient accuracy or inconsistencies of the on-ground calibration data, scan mirror degradation and stress induced changes of the polarization response of components inside the optical bench of the instrument. It is shown that it should in principle be feasible to recalibrate the effective polarization sensitivity of the instrument using the in-flight data and VRTM simulations.

Description: Evaluating calibration strategies for isotope ratio infrared spectroscopy for atmospheric 13 CO 2 / 12 CO 2 measurement Atmospheric Measurement Techniques, 6, 1491-1501, 2013 Author(s): X.-F. Wen, Y. Meng, X.-Y. Zhang, X.-M. Sun, and X. Lee Isotope ratio infrared spectroscopy (IRIS) provides an in situ technique for measuring δ 13 C in atmospheric CO 2 . A number of methods have been proposed for calibrating the IRIS measurements, but few studies have systematically evaluated their accuracy for atmospheric applications. In this study, we carried out laboratory and ambient measurements with two commercial IRIS analyzers and compared the accuracy of four calibration strategies. We found that calibration based on the 12 C and 13 C mixing ratios (Bowling et al., 2003) and on linear interpolation of the measured delta using the mixing ratio of the major isotopologue (Lee et al., 2005) yielded accuracy better than 0.06‰. Over a 7-day atmospheric measurement in Beijing, the two analyzers agreed to within −0.02 ± 0.18‰ after proper calibration. However, even after calibration the difference between the two analyzers showed a slight correlation with concentration, and this concentration dependence propagated through the Keeling analysis, resulting in a much larger difference of 2.44‰ for the Keeling intercept. The high sensitivity of the Keeling analysis to the concentration dependence underscores the challenge of IRIS for atmospheric research.

Description: Cavity ring-down spectroscopy sensor development for high-time-resolution measurements of gaseous elemental mercury in ambient air Atmospheric Measurement Techniques, 6, 1477-1489, 2013 Author(s): A. Pierce, D. Obrist, H. Moosmüller, X. Faïn, and C. Moore We describe further development of a previous laboratory prototype pulsed cavity ring-down spectroscopy (CRDS) sensor into a field-deployable system for high-time-resolution, continuous, and automated measurement of gaseous elemental mercury (GEM) concentrations in ambient air. We employed an external, isotopically enriched Hg cell for automated locking and stabilization of the laser wavelength on the GEM peak absorption during measurements. Further, we describe implementation of differential absorption measurements via a piezoelectric tuning element for pulse-by-pulse tuning of the laser wavelength onto and off of the GEM absorption line. This allowed us to continuously correct (at 25 Hz) for system baseline extinction losses unrelated to GEM absorption. Extensive measurement and calibration data obtained with the system were based on spike addition in both GEM-free air and ambient air. Challenges and interferences that occurred during measurements (particularly in ambient air) are discussed including temperature and ozone (O 3 ) concentration fluctuations, and steps taken to reduce these. CRDS data were highly linear ( r 2 ≥ 0.98) with data from a commercial Tekran 2537 Hg analyzer across a wide range of GEM concentrations (0 to 127 ng m −3 ) in Hg-free and ambient air. Measurements during periods of stable background GEM concentrations provided a conservative instrument sensitivity estimate of 0.35 ng m −3 for the CRDS system when time averaged for 5 min. This sensitivity, along with concentration patterns observed in ambient air (with the CRDS system and verified with the Tekran analyzer), showed that the sensor was capable of characterizing GEM fluctuations in ambient air. The value of fast-response GEM measurements was shown by a series of GEM spike additions – highlighting that high-temporal-resolution measurement allowed for detailed characterization of fast concentration fluctuations not possible with traditional analyzers.

Description: Chronology of Lake El'gygytgyn sediments Climate of the Past Discussions, 9, 3061-3102, 2013 Author(s): N. R. Nowaczyk, E. M. Haltia, D. Ulbricht, V. Wennrich, M. A. Sauerbrey, P. Rosén, H. Vogel, A. Francke, C. Meyer-Jacob, A. A. Andreev, and A. V. Lozhkin A 318 m long sedimentary profile drilled by the International Continental Scientific Drilling Program (ICDP) at Site 5011-1 in Lake El'gygytgyn, Far East Russian Arctic, has been analysed for its sedimentologic response to global climate modes by chrono-stratigraphic methods. The 12 km wide lake is sited in an 18 km large crater that was created by the impact of a meteorite 3.58 Ma ago. Since then sediments have been continuously deposited. For establishing their chronology, major reversals of the Earth's magnetic field provided initial tie points for the age model, confirming that the impact occurred in the earliest Gauss chron. Various stratigraphic parameters, reflecting redox conditions at the lake floor and climatic conditions in the catchment were tuned synchronously to Northern Hemisphere insolation variations and the marine oxygen isotope stack, respectively. Thus, a robust age model comprising more than 600 tie points could be defined. It could be shown that deposition of sediments in Lake El'gygytgyn occurred in concert with global climatic cycles. The upper ~160 m of sediments represent the past 3.3 Ma, equivalent to sedimentation rates of 4 to 5 cm ka −1 , whereas the lower 160 m represent just the first 0.3 Ma after the impact, equivalent to sedimentation rates in the order of 45 cm ka −1 .

Description: Late Cenozoic continuous aridification in the western Qaidam Basin: evidence from sporopollen records Climate of the Past Discussions, 9, 1485-1508, 2013 Author(s): Y. F. Miao, X. M. Fang, F. L. Wu, M. T. Cai, C. H. Song, Q. Q. Meng, and L. Xu Cenozoic climate changes in inner Asia provide a basis for understanding linkages between global cooling, the Tibetan Plateau uplift, and possibly the development of the East Asian monsoon. Based on the compiled palynological results from the western Qaidam Basin, this study reconstructed an 18 Ma record of changing vegetation and paleoclimates since the middle Miocene. Thermophilic taxa percentages were highest between 18 and 14 Ma and decreased after 14 Ma, corresponding closely with the Middle Miocene Climatic Optimum (MMCO) between 18 and 14 Ma and the following global climatic cooling. After 3.6 Ma, the thermophilic taxa percentages further decreased, showing the inevitable relations with the ice-sheets enlargement in the North Hemisphere. During the same period of time, the increase in xerophytic taxa percentages and decrease in conifers percentages imply aridification in both the basin and surrounding mountains since 18 Ma. These results indicate that global cooling mainly controlled the climate change from a relative warm-wet stage to a cold-dry stage during the late Cenozoic at the western Qaidam Basin, and that the Tibetan Plateau uplift also contributed in contrast to the East Asian summer monsoon.

Description: Post-Pliocene establishment of the present monsoonal climate in SW China: evidence from the late Pliocene Longmen megaflora Climate of the Past Discussions, 9, 1675-1701, 2013 Author(s): T. Su, F. M. B. Jacques, R. A. Spicer, Y.-S. Liu, Y.-J. Huang, Y.-W. Xing, and Z.-K. Zhou The paleoclimate of the late Pliocene Longmen flora from Yongping County located at the southeastern boundary of the Qinghai-Tibet Plateau was reconstructed using two leaf physiognomy based methods, i.e. Leaf Margin Analysis (LMA) and Climate Leaf Analysis Multivariate Program (CLAMP), to understand the paleoclimate condition and geographical pattern of monsoonal climate in southwestern China during the late Pliocene. The mean annual temperatures (MATs) estimated by LMA and CLAMP are 17.4 ± 3.3 °C and 17.4 ± 1.3 °C, respectively, compared with 15.9 °C at present. Meanwhile, the growing season precipitation (GSP) estimated by CLAMP is 1735.5 ± 217.7 mm in the Longmen flora, compared with 986.9 mm nowadays. The calculated monsoon index (MSI) of the Longmen flora is significantly lower than that of today. These results appear consistent with previous studies based on the coexistence approach (CA), and further suggest that there was a slightly warmer and much wetter climate during the late Pliocene than the present climate in western Yunnan. We conclude that the significant change of the monsoonal climate might have been resulted from the continuous uplift of mountains in western Yunnan, as well as the intensification of eastern Asian winter monsoon, both occurring concurrently in the post-Pliocene period.

Description: Holocene vegetation and climate changes in central Mediterranean inferred from a high-resolution marine pollen record (Adriatic Sea) Climate of the Past Discussions, 9, 1969-2014, 2013 Author(s): N. Combourieu-Nebout, O. Peyron, V. Bout-Roumazeilles, S. Goring, I. Dormoy, S. Joannin, L. Sadori, G. Siani, and M. Magny To understand the effects of future climate change on the ecology of the central Mediterranean we can look to the impacts of long-term, millennial to centennial-scale climatic variability on vegetation in the basin. Pollen data from the Adriatic Marine core MD 90-917 allows us to reconstruct vegetation and regional climate changes over the south central Mediterranean during the Holocene. Clay mineral ratios from the same core reflect the relative contributions of riverine (illite and smectite) and eolian (kaolinite) contributions to the site, and thus act as an additional proxy with which to test precipitation changes in the Holocene. Vegetation reconstruction shows vegetation responses to the late-Glacial Preboreal oscillation, most likely driven by changes in seasonal precipitation. Pollen-inferred temperature declines during the early-mid Holocene, but increases during the mid-late Holocene, similar to southern-western Mediterranean climatic patterns during the Holocene. Several short climatic events appear in the record, indicating the sensitivity of vegetation in the region to millennial-scale variability. Reconstructed summer precipitation shows a regional maximum between 8000 and 7000 cal yr BP similar to the general pattern across southern Europe. Two important shifts in vegetation occur at 7700 and between 7500 and 7000 yr. These vegetation shifts are linked to changes in seasonal precipitation and are correlated to increased river inputs respectively from the north (7700 event) and from the central Adriatic borderlands (7500–7000 event). These results reinforce the strengths of multi-proxy analysis and provide a deeper understanding of the role of precipitation and particularly the seasonality of precipitation in mediating vegetation change in the central Mediterranean during the Holocene.

Description: Southern Hemisphere orbital forcing and its effects on CO 2 and tropical Pacific climate Climate of the Past Discussions, 9, 1869-1900, 2013 Author(s): K. Tachikawa, A. Timmermann, L. Vidal, C. Sonzogni, and O. E. Timm The western Pacific warm pool (WPWP) is an important heat source for the atmospheric circulation and influences climate conditions worldwide. Understanding its sensitivity to past radiative perturbations may help better contextualize the magnitudes and patterns of current and projected tropical climate change. Here we present a new Mg/Ca-based sea surface temperature (SST) reconstruction over the past 400 kyr from the Bismarck Sea, off Papua New Guinea, along with results from a transient earth system model simulation. Our results document the primary influence of CO 2 forcing on glacial/interglacial WPWP SSTs and secondary effects due to changes in wind-driven tropical boundary currents. In addition to the SST, deep ocean temperature reconstructions from this core are linked with Southern Ocean temperature and sea-ice variations on timescales of ~ 23 kyr. It is proposed that Southern Hemisphere insolation changes serve as pacemaker for sea-ice variations in the Southern Ocean, which in turn modulate windstress curl-driven upwelling of carbon-rich waters, hence controlling atmospheric CO 2 and tropical WPWP temperatures.

Description: A regional climate palaeosimulation for Europe in the period 1500–1990 – Part 1: Model validation Climate of the Past Discussions, 9, 1803-1839, 2013 Author(s): J. J. Gómez-Navarro, J. P. Montávez, S. Wagner, and E. Zorita We present and analyse a high-resolution regional climate palaeosimulation encompassing the European region for the period 1500–1990. We use the regional model MM5 coupled to the global model ECHO-G. Both models were driven by reconstructions of three external factors: greenhouse gas concentrations, Total Solar Irradiance and volcanic activity. The simulation has been assessed in a recent period by comparing the model results with the Climate Research Unit (CRU) database. The results show that although the regional model is tightly driven by the boundary conditions, it is able to improve the reliability of the simulations, narrowing the differences to the observations, especially in areas of complex topography. Additionally, the evolution of the spatial distributions of temperature and precipitation through the last five centuries has been analysed. The mean values of temperature reflects the influence of the external forcings but, contrary to the results obtained under climate change scenario conditions, we found that higher-order momenta of the probability distribution of seasonal temperature and precipitation are hardly affected by changes in the external forcings

Description: North–south palaeohydrological contrasts in the central Mediterranean during the Holocene: tentative synthesis and working hypotheses Climate of the Past Discussions, 9, 1901-1967, 2013 Author(s): M. Magny, N. Combourieu Nebout, J. L. de Beaulieu, V. Bout-Roumazeilles, D. Colombaroli, S. Desprat, A. Francke, S. Joannin, O. Peyron, M. Revel, L. Sadori, G. Siani, M. A. Sicre, S. Samartin, A. Simonneau, W. Tinner, B. Vannière, B. Wagner, G. Zanchetta, F. Anselmetti, E. Brugiapaglia, E. Chapron, M. Debret, M. Desmet, J. Didier, L. Essallami, D. Galop, A. Gilli, J. N. Haas, N. Kallel, L. Millet, A. Stock, J. L. Turon, and S. Wirth On the basis of a multi-proxy approach and a strategy combining lacustrine and marine records along a north–south transect, data collected in the Central Mediterranean within the framework of a collaborative project have led to reconstruction of high-resolution and well-dated palaeohydrological records and to assessment of their spatial and temporal coherency. Contrasting patterns of palaeohydrological changes have been evidenced in the Central Mediterranean: south (north) of around 40° N of latitude, the middle part of the Holocene was characterised by lake-level maxima (minima), during an interval dated to ca. 10 300–4500 cal BP to the south and 9000–4500 cal BP to the north. Available data suggest that these contrasting palaeohydrological patterns operated throughout the Holocene, both on millennial and centennial scales. Regarding precipitation seasonality, maximum humidity in the Central Mediterranean during the middle part of the Holocene was characterised by humid winters and dry summers north of ca. 40° N, and humid winters and summers south of ca. 40° N. This may explain an apparent conflict between palaeoclimatic records depending on the proxies used for reconstruction as well as the synchronous expansion of tree species taxa with contrasting climatic requirements. In addition, south of ca. 40° N, the first millennium of the Holocene was characterised by very dry climatic conditions not only in the Eastern, but also in the Central and the Western Mediterranean zones as reflected by low lake levels and delayed reforestation. These results suggest that, in addition to the influence of the Nile discharge reinforced by the African monsoon, the deposition of Sapropel 1 has been favoured (1) by an increase in winter precipitation in the northern Mediterranean borderlands, and (2) by an increase in winter and summer precipitation in the southern Mediterranean area. The climate reversal following the Holocene climate optimum appears to have been punctuated by two major climate changes around 7500 and 4500 cal BP. In the Central Mediterranean, the Holocene palaeohydrological changes developed in response to a combination of orbital, ice-sheet and solar forcing factors. The maximum humidity interval in the south-central Mediterranean started at ca. 10 300 cal BP, in correlation with the decline (1) of the possible blocking effects of the North Atlantic anticyclone linked to maximum insolation, and/or (2) of the influence of the remnant ice sheets and fresh water forcing in the North Atlantic Ocean. In the north-central Mediterranean, the lake-level minimum interval began only around 9000 cal BP when the Fennoscandian ice-sheet disappeared and a prevailing positive NAO-type circulation developed in the North Atlantic area. The major palaeohydrological oscillation around 4500–4000 cal BP may be a non-linear response to the gradual decrease, with additional key seasonal and interhemispherical changes, in insolation. On a centennial scale, the successive climatic events which punctuated the entire Holocene in the central Mediterranean coincided with cooling events associated with deglacial outbursts in the North Atlantic area and decreases in solar activity during the interval 11 700–7000 cal BP, and to a possible combination of NAO-type circulation and solar forcing since ca. 7000 cal BP onwards. Thus, regarding the centennial-scale climatic oscillations, the Mediterranean Basin appears to have been strongly linked to the North Atlantic area and affected by solar activity over the entire Holocene. In addition to model experiments, a better understanding of forcing factors and past atmospheric circulation patterns behind the Holocene palaeohydrological changes in the Mediterranean area will require further investigation to establish additional high-resolution and well-dated records in selected locations around the Mediterranean Basin and in adjacent regions. Special attention should be paid to greater precision in the reconstruction, on millennial and centennial time scales, of changes in the latitudinal location of the limit between the northern and southern palaeohydrological Mediterranean sectors, depending on (1) the intensity and/or characteristics of climatic periods/oscillations (e.g. Holocene thermal maximum versus Neoglacial, as well as, for instance, the 8.2 ka event versus the 4 ka event or the Little Ice Age), and (2) on varying geographical conditions from the western to the eastern Mediterranean areas (longitudinal gradients).

Description: The last 7 millennia of vegetation and climate changes at Lago di Pergusa (central Sicily, Italy) Climate of the Past Discussions, 9, 2059-2094, 2013 Author(s): L. Sadori, E. Ortu, O. Peyron, G. Zanchetta, B. Vannière, M. Desmet, and M. Magny The aim of this study is to investigate climate changes and human activities under the lens of palynology. Based on a new high-resolution pollen sequence (PG2) from Lago di Pergusa (667 m a.s.l., central Sicily, Italy) covering the last 6700 yr, we propose a reconstruction of climate and landscape changes over the recent past in central Sicily. Compared to former studies from Lago di Pergusa (Sadori and Narcisi, 2001), this work provides a reconstruction of the evolution of vegetation and climate over the last millennia in central Sicily, indeed completing previous results with new data which is particularly detailed on the last 3000 yr. Joint actions of increasing dryness, climate oscillations, and human impact shaped the landscape of this privileged site. Lago di Pergusa, in fact, besides being the main inland lake of Sicily, is very sensitive to climate change and its territory was inhabited and exploited continuously since the prehistory. The lake sediments turned out to be a good observatory for the natural phenomena occurred in the last thousands of years. Results of the pollen-based study are integrated with changes in magnetic susceptibility and a tephra layer characterization. The tephra layer was shown to be related to the Sicanians' event, radiocarbon dated at 3055 ± 75 yr BP (Sadori and Narcisi, 2001). We performed palaeoclimate reconstructions by MAT and WA-PLS. Palaeoclimate reconstructions based on the core show important climate fluctuations throughout the Holocene. Climate reconstruction points out four phases of cooling and enhanced wetness in the last three millennia (2600–2000, 1650–1100, 850–550, 400–200 cal BP). This appears to be the evidence of local responses to global climate oscillations during the recent past.

Description: Broadband measurements of aerosol extinction in the ultraviolet spectral region Atmospheric Measurement Techniques, 6, 861-877, 2013 Author(s): R. A. Washenfelder, J. M. Flores, C. A. Brock, S. S. Brown, and Y. Rudich Aerosols influence the Earth's radiative budget by scattering and absorbing incoming solar radiation. The optical properties of aerosols vary as a function of wavelength, but few measurements have reported the wavelength dependence of aerosol extinction cross sections and complex refractive indices. We describe a new laboratory instrument to measure aerosol optical extinction as a function of wavelength, using cavity enhanced spectroscopy with a broadband light source. The instrument consists of two broadband channels which span the 360–390 and 385–420 nm spectral regions using two light emitting diodes (LED) and a grating spectrometer with charge-coupled device (CCD) detector. We determined aerosol extinction cross sections and directly observed Mie scattering resonances for aerosols that are purely scattering (polystyrene latex spheres and ammonium sulfate), slightly absorbing (Suwannee River fulvic acid), and strongly absorbing (nigrosin dye). We describe an approach for retrieving refractive indices as a function of wavelength from the measured extinction cross sections over the 360–420 nm wavelength region. The retrieved refractive indices for PSL and ammonium sulfate agree within uncertainty with the literature values for this spectral region. The refractive index determined for nigrosin is 1.78 (± 0.03) + 0.19 (± 0.08) i at 360 nm and 1.63 (± 0.03) + 0.21 (± 0.05) i at 420 nm. The refractive index determined for Suwannee River fulvic acid is 1.71 (± 0.02) + 0.07 (± 0.06) i at 360 nm and 1.66 (± 0.02) + 0.06 (± 0.04) i at 420 nm. These laboratory results support the potential for a field instrument capable of determining ambient aerosol optical extinction, average aerosol extinction cross section, and complex refractive index as a function of wavelength.

Description: Dust and associated trace element fluxes in a firn core from the coastal East Antarctica and its linkages with the Southern Hemisphere climate variability over the last ~ 50 yr Climate of the Past Discussions, 9, 1841-1867, 2013 Author(s): C. M. Laluraj, M. Thamban, and K. Satheesan High-resolution records of dust and trace element fluxes were studied in a firn core from the coastal Dronning Maud Land (cDML) in East Antarctica to identify the influence of climate variability on accumulation of these components over the past ~ 50 yr. A doubling of dust deposition was observed since 1985, coinciding with a shift in the Southern Annular Mode (SAM) index to positive values and associated increase in the wind speed. Back-trajectories showed that an increase in dust deposition is associated with the air parcels originating from north-west of the site, possibly indicating its origin from the Patagonian region. Our results suggest that while multiple processes could have influenced the increased dust formation, shift in SAM had a dominant influence on its transport. It is observed that since the 1985s the strength of easterlies increased significantly over the cDML region, which could sink air and dust material to the region that were brought by the westerlies through mass compensation. The correlation between the dust flux and δ 18 O records further suggest that enhanced dust flux in the firn core occurred during periods of colder atmospheric temperature, which reduced the moisture content and increased dust fall. Interestingly, the timing and amplitude of the insoluble dust peaks matched remarkably well with the fluxes of Ba, Cr, Cu, and Zn confirming that dust was the main carrier/source of atmospheric trace elements to East Antarctica during the recent past.

Description: Climatologies from satellite measurements: the impact of orbital sampling on the standard error of the mean Atmospheric Measurement Techniques, 6, 937-948, 2013 Author(s): M. Toohey and T. von Clarmann Climatologies of atmospheric observations are often produced by binning measurements according to latitude and calculating zonal means. The uncertainty in these climatological means is characterised by the standard error of the mean (SEM). However, the usual estimator of the SEM, i.e., the sample standard deviation divided by the square root of the sample size, holds only for uncorrelated randomly sampled measurements. Measurements of the atmospheric state along a satellite orbit cannot always be considered as independent because (a) the time-space interval between two nearest observations is often smaller than the typical scale of variations in the atmospheric state, and (b) the regular time-space sampling pattern of a satellite instrument strongly deviates from random sampling. We have developed a numerical experiment where global chemical fields from a chemistry climate model are sampled according to real sampling patterns of satellite-borne instruments. As case studies, the model fields are sampled using sampling patterns of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) and Atmospheric Chemistry Experiment Fourier-Transform Spectrometer (ACE-FTS) satellite instruments. Through an iterative subsampling technique, and by incorporating information on the random errors of the MIPAS and ACE-FTS measurements, we produce empirical estimates of the standard error of monthly mean zonal mean model O 3 in 5° latitude bins. We find that generally the classic SEM estimator is a conservative estimate of the SEM, i.e., the empirical SEM is often less than or approximately equal to the classic estimate. Exceptions occur only when natural variability is larger than the random measurement error, and specifically in instances where the zonal sampling distribution shows non-uniformity with a similar zonal structure as variations in the sampled field, leading to maximum sensitivity to arbitrary phase shifts between the sample distribution and sampled field. The occurrence of such instances is thus very sensitive to slight changes in the sampling distribution, and to the variations in the measured field. This study highlights the need for caution in the interpretation of the oft-used classically computed SEM, and outlines a relatively simple methodology that can be used to assess one component of the uncertainty in monthly mean zonal mean climatologies produced from measurements from satellite-borne instruments.

Description: An inter-laboratory investigation of the Arctic sea ice biomarker proxy IP 25 in marine sediments: key outcomes and recommendations Climate of the Past Discussions, 9, 5263-5298, 2013 Author(s): S. T. Belt, T. A. Brown, L. Ampel, P. Cabedo-Sanz, K. Fahl, J. J. Kocis, G. Massé, A. Navarro-Rodriguez, J. Ruan, and Y. Xu We describe the results of an inter-laboratory investigation into the identification and quantification of the Arctic sea ice biomarker proxy IP 25 in marine sediments. 7 laboratories took part in the study, which consisted of the analysis of IP 25 in a series of sediment samples from different regions of the Arctic, sub-Arctic and Antarctic, additional sediment extracts and purified standards. The results obtained allowed 4 key outcomes to be determined. First, IP 25 was identified by all laboratories in sediments from the Canadian Arctic with inter-laboratory variation in IP 25 concentration being substantially larger than within individual laboratories. This greater variation between laboratories was attributed to the difficulty in accurately determining instrumental response factors for IP 25 , despite provision of appropriate standards. Second, the identification of IP 25 by 3 laboratories in sediment from SW Iceland that was believed to represent a blank, was interpreted as representing a better limit of detection or quantification for such laboratories, contamination or mis-identification. These alternatives could not be distinguished conclusively with the data available, although it is noted that the precision of these data was significantly poorer compared with the other IP 25 concentration measurements. Third, 3 laboratories reported the occurrence of IP 25 in a sediment sample from the Antarctic Peninsula even though this biomarker is believed to be absent from the Southern Ocean. This anomaly is attributed to a combined chromatographic and mass spectrometric interference that results from the presence of a di-unsaturated highly branched isoprenoid (HBI) pseudo-homologue of IP 25 that occurs in Antarctic sediments. Finally, data are presented that suggest that extraction of IP 25 is consistent between Automated Solvent Extraction (ASE) and sonication methods and that IP 25 concentrations based on 7-hexylnonadecane as an internal standard are comparable using these methods. Recoveries of some more unsaturated HBIs and the internal standard 9-octylheptadecene, however, were lower with the ASE procedure, possibly due to partial degradation of these more reactive chemicals as a result of higher temperatures employed with this method. For future measurements, we recommend the use of reference sediment material with known concentration(s) of IP 25 for determining and routinely monitoring instrumental response factors. Given the significance placed on the presence (or otherwise) of IP 25 in marine sediments, some further recommendations pertaining to quality control are made that should also enable the two main anomalies identified here to be addressed.

Description: Expressions of climate perturbations in western Ugandan crater lake sediment records during the last 1000 yr Climate of the Past Discussions, 9, 5183-5226, 2013 Author(s): K. Mills, D. B. Ryves, N. J. Anderson, C. L. Bryant, and J. J. Tyler Equatorial East Africa has a complex, regional patchwork of climate regimes, with multiple interacting drivers. Recent studies have focussed on large lakes and reveal signals that are smoothed in both space and time, and, whilst useful at a continental scale, are of less relevance when understanding short-term, abrupt or immediate impacts of climate and environmental changes. Smaller-scale studies have highlighted spatial complexity and regional heterogeneity of tropical palaeoenvironments in terms of responses to climatic forcing (e.g. the Little Ice Age [LIA]) and questions remain over the spatial extent and synchroneity of climatic changes seen in East African records. Sediment cores from paired crater lakes in western Uganda were examined to assess ecosystem response to long-term climate and environmental change as well as testing responses to multiple drivers using redundancy analysis. These archives provide annual to sub-decadal records of environmental change. The records from the two lakes demonstrate an individualistic response to external (e.g. climatic) drivers, however, some of the broader patterns observed across East Africa suggest that the lakes are indeed sensitive to climatic perturbations such as a dry Mediaeval Climate Anomaly (MCA; 1000–1200 AD) and a relatively drier climate during the main phase of the LIA (1500–1800 AD); though lake levels in western Uganda do fluctuate. The relationship of Ugandan lakes to regional climate drivers breaks down c. 1800 AD, when major changes in the ecosystems appear to be a response to sediment and nutrient influxes as a result of increasing cultural impacts within the lake catchments. The data highlight the complexity of individual lake response to climate forcing, indicating shifting drivers through time. This research also highlights the importance of using multi-lake studies within a landscape to allow for rigorous testing of climate reconstructions, forcing and ecosystem response.

Description: A chemical analyzer for charged ultrafine particles Atmospheric Measurement Techniques, 6, 2339-2348, 2013 Author(s): S. G. Gonser and A. Held New particle formation is a frequent phenomenon in the atmosphere and of major significance for the Earth's climate and human health. To date the mechanisms leading to the nucleation of particles as well as to aerosol growth are not completely understood. A lack of appropriate measurement equipment for online analysis of the chemical composition of freshly nucleated particles is one major limitation. We have developed a Chemical Analyzer for Charged Ultrafine Particles (CAChUP) capable of analyzing particles with diameters below 30 nm. A bulk of size-separated particles is collected electrostatically on a metal filament, resistively desorbed and subsequently analyzed for its molecular composition in a time of flight mass spectrometer. We report on technical details as well as characterization experiments performed with the CAChUP. Our instrument was tested in the laboratory for its detection performance as well as for its collection and desorption capabilities. The manual application of defined masses of camphene (C 10 H 16 ) to the desorption filament resulted in a detection limit between 0.5 and 5 ng, and showed a linear response of the mass spectrometer. Flow tube experiments of 25 nm diameter secondary organic aerosol from ozonolysis of alpha-pinene also showed a linear relation between collection time and the mass spectrometer's signal intensity. The resulting mass spectra from the collection experiments are in good agreement with published work on particles generated by the ozonolysis of alpha-pinene. A sensitivity study shows that the current setup of CAChUP is ready for laboratory measurements and for the observation of new particle formation events in the field.

Description: Comparison of AOD between CALIPSO and MODIS: significant differences over major dust and biomass burning regions Atmospheric Measurement Techniques, 6, 2391-2401, 2013 Author(s): X. Ma, K. Bartlett, K. Harmon, and F. Yu Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) provide global vertical profiles of aerosol optical properties for the first time. In this study, we employed about 6 yr (2006–2011) of CALIPSO level 3 monthly mean gridded aerosol optical depth (AOD) products (daytime and nighttime) for cloud-free conditions, to compare with the Moderate Resolution Imaging Spectroradiometer (MODIS) Terra/Aqua level 3 monthly mean AOD dataset for the same time period. While the spatial distribution and seasonal variability of CALIPSO AOD is generally consistent with that of MODIS, CALIPSO is overall lower than MODIS as MODIS has higher frequency than CALIPSO for most bins of AOD. The correlation between MODIS and CALIPSO is better over ocean than over land. We focused on four regions that have large systematic differences: two over dust regions (the Sahara and Northwest China) and two over biomass burning regions (South Africa and South America). It is found that CALIPSO AOD is significantly lower than MODIS AOD over dust regions during the whole time period, with a maximum difference of 0.3 over the Saharan region and 0.25 over Northwest China. For biomass burning regions, CALIPSO AOD is significantly higher than MODIS AOD over South Africa, with a maximum difference of 0.25. Additionally CALIPSO AOD is slightly higher than MODIS AOD over South America for most of the time period, with a few exceptions in 2006, 2007, and 2010, when biomass burning is significantly stronger than during other years. We analyzed the impact of the satellite spatial and temporal sampling issue by using level 2 CALIPSO and MODIS products, and these systematic differences can still be found. The results of this study indicate that systematic differences of CALIPSO relative to MODIS are closely associated with aerosol types, which vary by location and season. Large differences over dust and biomass burning regions may suggest that assumptions made in satellite retrievals, such as the assumed lidar ratios for CALIPSO retrievals over dust and biomass burning regions or the surface reflectance information and/or the aerosol model utilized by the MODIS algorithm, are not appropriate.

Description: Evaluation of seasonal climates of the Mediterranean and nothern Africa in the CMIP5 simulations Climate of the Past Discussions, 9, 5347-5389, 2013 Author(s): A. Perez-Sanz, G. Li, P. González-Sampériz, and S. P. Harrison We analyze the spatial expression of seasonal climates of the Mediterranean and northern Africa in pre-Industrial ( piControl ) and mid-Holocene ( midHolocene , 6 ka) simulations from the fifth phase of the Coupled Model Intercomparison Project (CMIP5). Modern observations show four distinct precipitation regimes characterized by differences in the seasonal distribution and total amount of precipitation: an equatorial band characterized by a double peak in rainfall, the monsoon zone characterized by summer rainfall, the desert characterized by low seasonality and total precipitation, and the Mediterranean zone characterized by summer drought. Most models correctly simulate the position of the Mediterranean and the equatorial climates in the piControl simulations, but over-estimate the extent of monsoon influence and underestimate the extent of desert. However, most models fail to reproduce the amount of precipitation in each zone. Model biases in the simulated magnitude of precipitation are unrelated to whether the models reproduce the correct spatial patterns of each regime. In the midHolocene , the models simulate a reduction in winter rainfall in the equatorial zone, and a northward expansion of the monsoon with a significant increase in summer and autumn rainfall. Precipitation is slightly increased in the desert, mainly in summer and autumn, with northward expansion of the monsoon. Changes in the Mediterranean are small, although there is an increase in spring precipitation consistent with palaeo-observations of increased growing-season rainfall. Comparison with reconstructions shows that most models under-estimate the mid-Holocene changes in annual precipitation, except in the equatorial zone. Biases in the piControl have only a limited influence on midHolocene anomalies in ocean-atmosphere models; carbon-cycle models show no relationship between piControl bias and midHolocene anomalies. Biases in the prediction of the midHolocene monsoon expansion are unrelated to how well the models simulate changes in Mediterranean climate.

Description: Orbital and millennial-scale environmental changes between 64 and 25 ka BP recorded in Black Sea sediments Climate of the Past Discussions, 9, 5439-5477, 2013 Author(s): L. S. Shumilovskikh, D. Fleitmann, N. R. Nowaczyk, H. Behling, F. Marret, A. Wegwerth, and H. W. Arz High-resolution pollen and dinoflagellate cyst records from marine sediment core 25-GC1 were used to reconstruct vegetation dynamics in Northern Anatolia and surface conditions of the Black Sea between 64 and 25 ka BP. During this period, the dominance of Artemisia in the pollen record indicates a steppe landscape and arid climate conditions. However, the presence of temperate and warm-temperate arboreal pollen suggests the existence of glacial refugia in Northern Anatolia. A general cooling trend towards 25 ka BP is evidenced by the decrease of Quercus and increase of Pinus . There is evidence of orbital-driven vegetation dynamics in Northern Anatolia during 64–25 ka BP with spread of steppe during precession minima (insolation maxima) and development of forests during precession maxima (insolation minima). Dansgaard–Oeschger (D–O) events are characterized by a marked increase in temperate tree pollen, indicating a spread of forests due to warm and wet conditions in Northern Anatolia. The dominance of Pyxidinopsis psilata and Spiniferites cruciformis in the dinocyst record indicates a rather brackish Black Sea during the last glacial period. The decrease of marine indicators (marine dinocysts, acritachs) at ~ 54 ka BP and increase of freshwater algae ( Pediastrum, Botryococcus ) from 32 to 25 ka BP reveals freshening of the Black Sea surface water, related to orbital-driven arid/humid phases in the region, influencing hydrology and level changes of the Black Sea. D–O interstadials are characterized by high dinocyst concentrations and calcium carbonate content, as a result of an increase in primary productivity in the Black Sea. Heinrich events show a similar impact on the environment in Northern Anatolia/Black Sea region as D–O stadials.

Description: Microwave radiometer to retrieve temperature profiles from the surface to the stratopause Atmospheric Measurement Techniques, 6, 2477-2494, 2013 Author(s): O. Stähli, A. Murk, N. Kämpfer, C. Mätzler, and P. Eriksson TEMPERA (TEMPERature RAdiometer) is a new ground-based radiometer which measures in a frequency range from 51–57 GHz radiation emitted by the atmosphere. With this instrument it is possible to measure temperature profiles from ground to about 50 km. This is the first ground-based instrument with the capability to retrieve temperature profiles simultaneously for the troposphere and stratosphere. The measurement is done with a filterbank in combination with a digital fast Fourier transform spectrometer. A hot load and a noise diode are used as stable calibration sources. The optics consist of an off-axis parabolic mirror to collect the sky radiation. Due to the Zeeman effect on the emission lines used, the maximum height for the temperature retrieval is about 50 km. The effect is apparent in the measured spectra. The performance of TEMPERA is validated by comparison with nearby radiosonde and satellite data from the Microwave Limb Sounder on the Aura satellite. In this paper we present the design and measurement method of the instrument followed by a description of the retrieval method, together with a validation of TEMPERA data over its first year, 2012.

Description: Retrieval of nitric oxide in the mesosphere and lower thermosphere from SCIAMACHY limb spectra Atmospheric Measurement Techniques, 6, 2521-2531, 2013 Author(s): S. Bender, M. Sinnhuber, J. P. Burrows, M. Langowski, B. Funke, and M. López-Puertas We use the ultra-violet (UV) spectra in the range 230–300 nm from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) to retrieve the nitric oxide (NO) number densities from atmospheric emissions in the gamma-bands in the mesosphere and lower thermosphere. Using 3-D ray tracing, a 2-D retrieval grid, and regularisation with respect to altitude and latitude, we retrieve a whole semi-orbit simultaneously for the altitude range from 60 to 160 km. We present details of the retrieval algorithm, first results, and initial comparisons to data from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). Our results agree on average well with MIPAS data and are in line with previously published measurements from other instruments. For the time of available measurements in 2008–2011, we achieve a vertical resolution of 5–10 km in the altitude range 70–140 km and a horizontal resolution of about 9° from 60° S–60° N. With this we have independent measurements of the NO densities in the mesosphere and lower thermosphere with approximately global coverage. This data can be further used to validate climate models or as input for them.

Description: Development and field testing of a rapid and ultra-stable atmospheric carbon dioxide spectrometer Atmospheric Measurement Techniques, 7, 4445-4453, 2014 Author(s): B. Xiang, D. D. Nelson, J. B. McManus, M. S. Zahniser, R. A. Wehr, and S. C. Wofsy We present field test results for a new spectroscopic instrument to measure atmospheric carbon dioxide (CO 2 ) with high precision (0.02 μmol mol −1 , or ppm at 1 Hz) and demonstrate high stability (within 0.1 ppm over more than 8 months), without the need for hourly, daily, or even monthly calibration against high-pressure gas cylinders. The technical novelty of this instrument (ABsolute Carbon dioxide, ABC) is the spectral null method using an internal quartz reference cell with known CO 2 column density. Compared to a previously described prototype, the field instrument has better stability and benefits from more precise thermal control of the optics and more accurate pressure measurements in the sample cell (at the mTorr level). The instrument has been deployed at a long-term ecological research site (the Harvard Forest, USA), where it has measured for 8 months without on-site calibration and with minimal maintenance, showing drift bounds of less than 0.1 ppm. Field measurements agree well with those of a commercially available cavity ring-down CO 2 instrument (Picarro G2301) run with a standard calibration protocol. This field test demonstrates that ABC is capable of performing high-accuracy, unattended, continuous field measurements with minimal use of reference gas cylinders.

Description: Investigating uptake of N 2 O in agricultural soils using a high-precision dynamic chamber method Atmospheric Measurement Techniques, 7, 4455-4462, 2014 Author(s): N. J. Cowan, D. Famulari, P. E. Levy, M. Anderson, D. S. Reay, and U. M. Skiba Uptake (or negative flux) of nitrous oxide (N 2 O) in agricultural soils is a controversial issue which has proved difficult to investigate in the past due to constraints such as instrumental precision and methodological uncertainties. Using a recently developed high-precision quantum cascade laser gas analyser combined with a closed dynamic chamber, a well-defined detection limit of 4 μg N 2 O-N m −2 h −1 could be achieved for individual soil flux measurements. 1220 measurements of N 2 O flux were made from a variety of UK soils using this method, of which 115 indicated uptake by the soil (i.e. a negative flux in the micrometeorological sign convention). Only four of these apparently negative fluxes were greater than the detection limit of the method, which suggests that the vast majority of reported negative fluxes from such measurements are actually due to instrument noise. As such, we suggest that the bulk of negative N 2 O fluxes reported for agricultural fields are most likely due to limits in detection of a particular flux measurement methodology and not a result of microbiological activity consuming atmospheric N 2 O.

Description: Rapid, optical measurement of the atmospheric pressure on a fast research aircraft using open-path TDLAS Atmospheric Measurement Techniques, 7, 3653-3666, 2014 Author(s): B. Buchholz, A. Afchine, and V. Ebert Because of the high travel speed, the complex flow dynamics around an aircraft, and the complex dependency of the fluid dynamics on numerous airborne parameters, it is quite difficult to obtain accurate pressure values at a specific instrument location of an aircraft's fuselage. Complex simulations using computational fluid dynamics (CFD) models can in theory computationally "transfer" pressure values from one location to another. However, for long flight patterns, this process is inconvenient and cumbersome. Furthermore, these CFD transfer models require a local experimental validation, which is rarely available. In this paper, we describe an integrated approach for a spectroscopic, calibration-free, in-flight pressure determination in an open-path White cell on an aircraft fuselage using ambient, atmospheric water vapour as the "sensor species". The presented measurements are realised with the HAI (Hygrometer for Atmospheric Investigations) instrument, built for multiphase water detection via calibration-free TDLAS (tunable diode laser absorption spectroscopy). The pressure determination is based on raw data used for H 2 O concentration measurement, but with a different post-flight evaluation method, and can therefore be conducted at deferred time intervals on any desired flight track. The spectroscopic pressure is compared in-flight with the static ambient pressure of the aircraft avionic system and a micro-mechanical pressure sensor, located next to the open-path cell, over a pressure range from 150 to 800 hPa, and a water vapour concentration range of more than 3 orders of magnitude. The correlation between the micro-mechanical pressure sensor measurements and the spectroscopic pressure measurements shows an average deviation from linearity of only 0.14% and a small offset of 9.5 hPa. For the spectroscopic pressure evaluation we derive measurement uncertainties under laboratory conditions of 3.2 and 5.1% during in-flight operation on the HALO airplane. Under certain flight conditions we quantified, for the first time, stalling-induced, dynamic pressure deviations of up to 30% (at 200 hPa) between the avionic sensor and the optical and mechanical pressure sensors integrated in HAI. Such severe local pressure deviations from the typically used avionic pressure are important to take into account for other airborne sensors employed on such fast flying platforms as the HALO aircraft.

Description: Mixing-layer height retrieval with ceilometer and Doppler lidar: from case studies to long-term assessment Atmospheric Measurement Techniques, 7, 3685-3704, 2014 Author(s): J. H. Schween, A. Hirsikko, U. Löhnert, and S. Crewell Aerosol signatures observed by ceilometers are frequently used to derive mixing-layer height (MLH) which is an essential variable for air quality modelling. However, Doppler wind lidar measurements of vertical velocity can provide a more direct estimation of MLH via simple thresholding. A case study reveals difficulties in the aerosol-based MLH retrieval during transition times when the mixing layer builds up in the morning and when turbulence decays in the afternoon. The difficulties can be explained by the fact that the aerosol distribution is related to the history of the mixing process and aerosol characteristics are modified by humidification. The results of the case study are generalized by evaluating one year of joint measurements by a Vaisala CT25K and a HALO Photonics Streamline wind lidar. On average the aerosol-based retrieval gives higher MLH than the wind lidar with an overestimation of MLH by about 300 m (600 m) in the morning (late afternoon). Also, the daily aerosol-based maximum MLH is larger and occurs later during the day and the average morning growth rates are smaller than those derived from the vertical wind. In fair weather conditions classified by less than 4 octa cloud cover the mean diurnal cycle of cloud base height corresponds well to the mixing-layer height showing potential for a simplified MLH estimation.

Description: Radio occultation bending angle anomalies during tropical cyclones Atmospheric Measurement Techniques, 4, 1053-1060, 2011 Author(s): R. Biondi, T. Neubert, S. Syndergaard, and J. K. Nielsen The tropical deep convection affects the radiation balance of the atmosphere changing the water vapor mixing ratio and the temperature of the upper troposphere lower stratosphere. The aim of this work is to better understand these processes and to investigate if severe storms leave a significant signature in radio occultation profiles in the tropical tropopause layer. Using tropical cyclone best track database and data from different GPS radio occultation missions (COSMIC, GRACE, CHAMP, SACC and GPSMET), we selected 1194 profiles in a time window of 3 h and a space window of 300 km from the eye of the cyclone. We show that the bending angle anomaly of a GPS radio occultation signal is typically larger than the climatology in the upper troposphere and lower stratosphere and that a double tropopause during deep convection can easily be detected using this technique. Comparisons with co-located radiosondes, climatology of tropopause altitudes and GOES analyses are also shown to support the hypothesis that the bending angle anomaly can be used as an indicator of convective towers. The results are discussed in connection to the GPS radio occultation receiver which will be part of the Atomic Clock Ensemble in Space (ACES) payload on the International Space Station.

Description: Assimilation of GPS radio occultation data at DWD Atmospheric Measurement Techniques, 4, 1105-1113, 2011 Author(s): H. Anlauf, D. Pingel, and A. Rhodin We describe the status of the assimilation of bending angles from GPS radio occultations in the 3D-Var for DWD's operational global forecast model GME ("Global Model for Europe"). Experiments show that the assimilation of GPSRO data leads to a significant reduction of biases in the analyses of temperature, humidity and wind in the upper troposphere and the stratosphere, as well as a better r. m. s. fit in the comparison to radiosondes. The impact on forecasts is most prominent in the data sparse Southern Hemisphere, but is also quite notable in the Northern Hemisphere extra-tropics. The positive results found in the impact experiments lead to the implementation of the assimilation of GPS radio occultations from GRACE-A, FORMOSAT-3/COSMIC and GRAS/MetOp-A into the operational suite on 3 August 2010. We also show some initial results from assimilation experiments using radio occultation data from the German research satellite TerraSAR-X.

Description: Tropical climate and vegetation changes during Heinrich Event 1: comparing climate model output to pollen-based vegetation reconstructions with emphasis on the region around the tropical Atlantic Ocean Climate of the Past Discussions, 7, 1973-2019, 2011 Author(s): D. Handiani, A. Paul, and L. Dupont Abrupt climate changes associated with Heinrich Event 1 (HE1) about 18 to 15 thousand years before present (ka BP) strongly affected climate and vegetation patterns not only in the Northern Hemisphere, but also in tropical regions in the South Atlantic Ocean. We used the University of Victoria (UVic) Earth System-Climate Model (ESCM) with dynamical vegetation and land surface components to simulate four scenarios of climate-vegetation interaction: the pre-industrial era (PI), the Last Glacial Maximum (LGM), and a Heinrich-like event with two different climate backgrounds (interglacial and glacial). The HE1-like simulation with a glacial climate background produced sea surface temperature patterns and enhanced interhemispheric thermal gradients in accordance with the "bipolar seesaw" hypothesis. It allowed us to investigate the vegetation changes that result from a transition to a drier climate as predicted for northern tropical Africa due to a southward shift of the Intertropical Convergence Zone (ITCZ). We found that a cooling of the Northern Hemisphere caused a southward shift of those plant-functional types (PFTs) in Northern Tropical Africa that are indicative of an increased desertification, and a retreat of broadleaf forests in Western Africa and Northern South America. We used the PFTs generated by the model to calculate mega-biomes to allow for a direct comparison between paleodata and palynological vegetation reconstructions. Our calculated mega-biomes for the pre-industrial period and the LGM corresponded well to the modern and LGM sites of the BIOME6000 (v.4.2) reconstruction, except that our present-day simulation predicted the dominance of grassland in Southern Europe and our LGM simulation simulated more forest cover in tropical and sub-tropical South America. The mega-biomes from the HE1 simulation with glacial background climate were in agreement with paleovegetation data from land and ocean proxies in West, Central, and Northern Tropical Africa as well as Northeast South America. However, our model did not agree well with predicted biome distributions in Eastern South America.

Description: Bridging the Faraoni and Selli oceanic anoxic events: short and repetitive dys- and anaerobic episodes during the late Hauterivian to early Aptian in the central Tethys Climate of the Past Discussions, 7, 2021-2059, 2011 Author(s): K. B. Föllmi, M. Bôle, N. Jammet, P. Froidevaux, A. Godet, S. Bodin, T. Adatte, V. Matera, D. Fleitmann, and J. E. Spangenberg A detailed stratigraphical and geochemical analysis was performed on the upper part of the Maiolica Formation outcropping in the Breggia (southern Switzerland) and Capriolo sections (northern Italy). In these localities, the Maiolica Formation consists of well-bedded, partly siliceous, pelagic, micritic carbonate, which lodges numerous thin, dark and organic-rich layers. Stable-isotope, phosphorus, organic-carbon and a suite of redox-sensitive trace-metal contents (RSTE: Mo, U, Co, V and As) were measured. Higher densities of organic-rich layers were identified in the uppermost Hauterivian, lower Barremian and the Barremian-Aptian boundary intervals, whereas the upper Barremian interval and the interval immediately following the Barremian-Aptian boundary interval are characterized by lower densities of organic-rich layers. TOC contents, RSTE pattern and C org :P tot ratios indicate that most layers were deposited under dysaerobic rather than anaerobic conditions and that latter conditions were likely restricted to short intervals in the latest Hauterivian, the early Barremian and the pre-Selli early Aptian. Correlations are possible with organic-rich intervals in central Italy (the Gorgo a Cerbara section) and the Boreal northwest German Basin, and with the facies and drowning pattern in the evolution of the Helvetic segment of the northern Tethyan carbonate platform. Our data and correlations suggest that the latest Hauterivian witnessed the progressive installation of dysaerobic conditions in the Tethys, which went along with the onset in sediment condensation, phosphogenesis and platform drowning on the northern Tethyan margin, and which culminated in the Faraoni anoxic episode. This brief episode is followed by further episodes of dysaerobic conditions in the Tethys and the northwest German Basin, which became more frequent and progressively stronger in the late early Barremian. Platform drowning persisted and did not halt before the latest early Barremian. The late Barremian witnessed diminishing frequencies and intensities in dysaerobic conditions, which went along with the progressive installation of the Urgonian carbonate platform. Near the Barremian-Aptian boundary, the increasing density in dysaerobic episodes in the Tethyan and northwest German Basins is paralleled by a change towards heterozoan carbonate production on the northern Tethyan shelf. The following return to more oxygenated conditions is correlated with the second phase of Urgonian platform growth and the period immediately preceding and corresponding to the Selli anoxic episode is characterized by renewed platform drowning and the change to heterozoan carbonate production. Changes towards more humid climate conditions were likely the cause for the repetitive installation of dys- to anaerobic conditions in the Tethyan and Boreal basins and the accompanying changes in the evolution of the carbonate platform towards heterozoan carbonate-producing ecosystems and platform drowning.

Description: CIAO: the CNR-IMAA advanced observatory for atmospheric research Atmospheric Measurement Techniques, 4, 1191-1208, 2011 Author(s): F. Madonna, A. Amodeo, A. Boselli, C. Cornacchia, V. Cuomo, G. D'Amico, A. Giunta, L. Mona, and G. Pappalardo Long-term observations of aerosol and clouds are of crucial importance to understand the weather climate system. At the Istituto di Metodologie per l'Analisi Ambientale of the Italian National Research Council (CNR-IMAA) an advanced atmospheric observatory, named CIAO, is operative. CIAO (CNR-IMAA Atmospheric Observatory) main scientific objective is the long term measurement for the climatology of aerosol and cloud properties. Its equipment addresses the state-of-the-art for the ground-based remote sensing of aerosol, water vapour and clouds including active and passive sensors, like lidars, ceilometers, radiometers, and a radar. This paper describes the CIAO infrastructure, its scientific activities as well as the observation strategy. The observation strategy is mainly organized in order to provide quality assured measurements for satellite validation and model evaluation and to fully exploit the synergy and integration of the active and passive sensors for the improvement of atmospheric profiling. Data quality is ensured both by the application of protocols and dedicated quality assurance programs mainly related to the projects and networks in which the infrastructure is involved. The paper also introduces examples of observations performed at CIAO and of the synergies and integration algorithms (using Raman lidar and microwave profiler data) developed and implemented at the observatory for the optimization and improvement of water vapour profiling. CIAO database represents an optimal basis to study the synergy between different sensors and to investigate aerosol-clouds interactions, and can give a significant contribution to the validation programs of the incoming new generation satellite missions.

Description: Degree-day melt models for paleoclimate reconstruction from tropical glaciers: calibration from mass balance and meteorological data of the Zongo glacier (Bolivia, 16 ° S) Climate of the Past Discussions, 7, 2119-2158, 2011 Author(s): P.-H. Blard, P. Wagnon, J. Lavé, A. Soruco, J.-E. Sicart, and B. Francou This paper describes several simple positive degree-day models (hereafter referred as "PDD models") designed to provide past climatic reconstruction from tropical glacier paleo-equilibrium altitude lines (paleo-ELA). Several ablation laws were tested and calibrated using the monthly ablation and meteorological data recorded from 1997 to 2006 on the Zongo glacier (Cordillera Real, Bolivia, 16° S). The performed inversion analyses indicate that the model provides a better reconstruction of the mass balance if the ablation is modeled with different melting factors for snow and ice. The inclusion of short-wave solar radiations does not induce a substantial improvement. However, this type of model may be very useful to quantify the effects of local topographic (orientation, shading) and to take into account incoming solar radiation changes at geological timescale. The performed sensitivity test indicates that, in spite of the uncertainty in the calibrated snow-ice ablation factors, all models are able to provide paleotemperatures with ~1 °C uncertainty for a given paleoprecipitation. This error includes a 50 m uncertainty in the estimate of the paleoELA. Finally, the models are characterized by different precipitation-temperature sensitivities: if a similar warming is applied, model including different ablation factors for snow and ice requires a lower precipitation increase (by ∼15 %) than others to maintain the ELA.

Description: Airborne DOAS limb measurements of tropospheric trace gas profiles: case studies on the profile retrieval of O 4 and BrO Atmospheric Measurement Techniques, 4, 1241-1260, 2011 Author(s): C. Prados-Roman, A. Butz, T. Deutschmann, M. Dorf, L. Kritten, A. Minikin, U. Platt, H. Schlager, H. Sihler, N. Theys, M. Van Roozendael, T. Wagner, and K. Pfeilsticker A novel limb scanning mini-DOAS spectrometer for the detection of UV/vis absorbing radicals (e.g., O 3 , BrO, IO, HONO) was deployed on the DLR-Falcon (Deutsches Zentrum für Luft- und Raumfahrt) aircraft and tested during the ASTAR 2007 campaign (Arctic Study of Tropospheric Aerosol, Clouds and Radiation) that took place at Svalbard (78° N) in spring 2007. Our main objectives during this campaign were to test the instrument, and to perform spectral and profile retrievals of tropospheric trace gases, with particular interest on investigating the distribution of halogen compounds (e.g., BrO) during the so-called ozone depletion events (ODEs). In the present work, a new method for the retrieval of vertical profiles of tropospheric trace gases from tropospheric DOAS limb observations is presented. Major challenges arise from modeling the radiative transfer in an aerosol and cloud particle loaded atmosphere, and from overcoming the lack of a priori knowledge of the targeted trace gas vertical distribution (e.g., unknown tropospheric BrO vertical distribution). Here, those challenges are tackled by a mathematical inversion of tropospheric trace gas profiles using a regularization approach constrained by a retrieved vertical profile of the aerosols extinction coefficient E M . The validity and limitations of the algorithm are tested with in situ measured E M , and with an absorber of known vertical profile (O 4 ). The method is then used for retrieving vertical profiles of tropospheric BrO. Results indicate that, for aircraft ascent/descent observations, the limit for the BrO detection is roughly 1.5 pptv (pmol mol −1 ), and the BrO profiles inferred from the boundary layer up to the upper troposphere and lower stratosphere have around 10 degrees of freedom. For the ASTAR 2007 deployments during ODEs, the retrieved BrO vertical profiles consistently indicate high BrO mixing ratios (∼15 pptv) within the boundary layer, low BrO mixing ratios (≤1.5 pptv) in the free troposphere, occasionally enhanced BrO mixing ratios (∼1.5 pptv) in the upper troposphere, and increasing BrO mixing ratios with altitude in the lowermost stratosphere. These findings agree reasonably well with satellite and balloon-borne soundings of total and partial BrO atmospheric column densities.

Description: Processing of GRAS/METOP radio occultation data recorded in closed-loop and raw-sampling modes Atmospheric Measurement Techniques, 4, 1021-1026, 2011 Author(s): M. E. Gorbunov, K. B. Lauritsen, H.-H. Benzon, G. B. Larsen, S. Syndergaard, and M. B. Sørensen Instrument GRAS (Global Navigation Satellite System Receiver for Atmospheric Sounding) on-board of the Metop-A satellite was activated on 27 October 2006. Currently, Metop-A is a fully operational satellite with GRAS providing from 650–700 occultations per day. We describe our processing of GRAS data based on the modification of our OCC software, which was modified to become capable of reading and processing GRAS data. We perform a statistical comparison of bending angles and refractivities derived from GRAS data with those derived from ECMWF analyses. We conclude that GRAS data have error characteristics close to those of COSMIC data. In the height range 10–30 km, the systematic refractivity difference GRAS–ECMWF is of the order of 0.1–0.2 %, and the standard deviation is 0.3–0.6 %. In the lower troposphere GRAS refractivity and bending angle indicate a negative bias, which reaches its maximum value in the tropics. In particular the retrieved refractivity is biased by up to 2.5 %. The negative bias pattern is similar to that found in the statistical validation of COSMIC data. This makes it probable that the bias should not be attributed to the instrument design or hardware.

Description: Eight-component retrievals from ground-based MAX-DOAS observations Atmospheric Measurement Techniques, 4, 1027-1044, 2011 Author(s): H. Irie, H. Takashima, Y. Kanaya, K. F. Boersma, L. Gast, F. Wittrock, D. Brunner, Y. Zhou, and M. Van Roozendael We attempt for the first time to retrieve lower-tropospheric vertical profile information for 8 quantities from ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations. The components retrieved are the aerosol extinction coefficients at two wavelengths, 357 and 476 nm, and NO 2 , HCHO, CHOCHO, H 2 O, SO 2 , and O 3 volume mixing ratios. A Japanese MAX-DOAS profile retrieval algorithm, version 1 (JM1), is applied to observations performed at Cabauw, the Netherlands (51.97° N, 4.93° E), in June–July 2009 during the Cabauw Intercomparison campaign of Nitrogen Dioxide measuring Instruments (CINDI). Of the retrieved profiles, we focus here on the lowest-layer data (mean values at altitudes 0–1 km), where the sensitivity is usually highest owing to the longest light path. In support of the capability of the multi-component retrievals, we find reasonable overall agreement with independent data sets, including a regional chemical transport model (CHIMERE) and in situ observations performed near the surface (2–3 m) and at the 200-m height level of the tall tower in Cabauw. Plumes of enhanced HCHO and SO 2 were likely affected by biogenic and ship emissions, respectively, and an improvement in their emission strengths is suggested for better agreement between CHIMERE simulations and MAX-DOAS observations. Analysis of air mass factors indicates that the horizontal spatial representativeness of MAX-DOAS observations is about 3–15 km (depending mainly on aerosol extinction), comparable to or better than the spatial resolution of current UV-visible satellite observations and model calculations. These demonstrate that MAX-DOAS provides multi-component data useful for the evaluation of satellite observations and model calculations and can play an important role in bridging different data sets having different spatial resolutions.

Description: Deglaciation records of 17 O- excess in East Antarctica: reliable reconstruction of oceanic relative humidity from coastal sites Climate of the Past Discussions, 7, 1845-1886, 2011 Author(s): R. Winkler, A. Landais, H. Sodemann, L. Dümbgen, F. Prié, V. Masson-Delmotte, B. Stenni, and J. Jouzel We measured δ 17 O and δ 18 O in two Antarctic ice cores at EPICA Dome C (EDC) and TALDICE (TD), respectively and computed 17 O- excess with respect to VSMOW. The comparison of our 17 O- excess data with the previous record obtained at Vostok (Landais et al., 2008) revealed differences up to 35 ppm in 17 O- excess mean level and evolution for the three sites. Our data showed that the large increase depicted at Vostok (20 ppm) during the last deglaciation, is a regional and not a general pattern in the temporal distribution of 17 O- excess in East Antarctica. The EDC data display an increase of 13 ppm, whereas the TD data show no significant variation from the Last Glacial Maximum (LGM) to the Early Holocene (EH). Lagrangian moisture source diagnostic revealed very different source regions for Vostok and EDC compared to TD. These findings combined with the results of a sensitivity analysis, using a Rayleigh-type isotopic model, suggest that relative humidity (RH) at the oceanic source region (OSR) are a determining factor for the spatial differences of 17 O- excess in East Antarctica. However, 17 O- excess in remote sites of continental Antarctica (e.g. Vostok) may be highly sensitive to local effects. Hence, we consider 17 O- excess in coastal East Antarctic ice cores (TD) to be more reliable as a proxy for RH at the OSR.

Description: Impact of oceanic processes on the carbon cycle during the last termination Climate of the Past Discussions, 7, 1887-1934, 2011 Author(s): N. Bouttes, D. Paillard, D. M. Roche, C. Waelbroeck, M. Kageyama, A. Lourantou, E. Michel, and L. Bopp During the last termination (from ~18 000 yr ago to ~9000 yr ago) the climate significantly warmed and the ice sheets melted. Simultaneously, atmospheric CO 2 increased from ~190 ppm to ~260 ppm. Although this CO 2 rise plays an important role in the deglacial warming, the reasons for its evolution are difficult to explain. Only box models have been used to run transient simulations of this carbon cycle transition, but by forcing the model with data constrained scenarios of the evolution of temperature, sea level, sea ice, NADW formation, Southern Ocean vertical mixing and biological carbon pump. More complex models (including GCMs) have investigated some of these mechanisms but they have only been used to try and explain LGM versus present day steady-state climates. In this study we use a climate-carbon coupled model of intermediate complexity to explore the role of three oceanic processes in transient simulations: the sinking of brines, stratification-dependant diffusion and iron fertilization. Carbonate compensation is accounted for in these simulations. We show that neither iron fertilization nor the sinking of brines alone can account for the evolution of CO 2 , and that only the combination of the sinking of brines and interactive diffusion can simultaneously simulate the increase in deep Southern Ocean δ 13 C. The scenario that agrees best with the data takes into account all mechanisms and favours a rapid cessation of the sinking of brines around 18 000 yr ago, when the Antarctic ice sheet extent was at its maximum. Sea ice formation was then shifted to the open ocean where the salty water is quickly mixed with fresher water, which prevents deep sinking of salty water and therefore breaks down the deep stratification and releases carbon from the abyss. Based on this scenario it is possible to simulate both the amplitude and timing of the CO 2 increase during the last termination in agreement with data. The atmospheric δ 13 C appears to be highly sensitive to changes in the terrestrial biosphere, underlining the need to better constrain the vegetation evolution during the termination.

Description: Preliminary validation of column-averaged volume mixing ratios of carbon dioxide and methane retrieved from GOSAT short-wavelength infrared spectra Atmospheric Measurement Techniques, 4, 1061-1076, 2011 Author(s): I. Morino, O. Uchino, M. Inoue, Y. Yoshida, T. Yokota, P. O. Wennberg, G. C. Toon, D. Wunch, C. M. Roehl, J. Notholt, T. Warneke, J. Messerschmidt, D. W. T. Griffith, N. M. Deutscher, V. Sherlock, B. Connor, J. Robinson, R. Sussmann, and M. Rettinger Column-averaged volume mixing ratios of carbon dioxide and methane retrieved from the Greenhouse gases Observing SATellite (GOSAT) Short-Wavelength InfraRed observation (GOSAT SWIR X CO 2 and X CH 4 ) were compared with the reference calibrated data obtained by ground-based high-resolution Fourier Transform Spectrometers (g-b FTSs) participating in the Total Carbon Column Observing Network (TCCON). Preliminary results are as follows: the GOSAT SWIR X CO 2 and X CH 4 (Version 01.xx) are biased low by 8.85 ± 4.75 ppm (2.3 ± 1.2 %) and 20.4 ± 18.9 ppb (1.2 ± 1.1 %), respectively. The standard deviation of the GOSAT SWIR X CO 2 and X CH 4 is about 1 % (1 σ) after correcting the negative biases of X CO 2 and X CH 4 by 8.85 ppm and 20.4 ppb, respectively. The latitudinal distributions of zonal means of the GOSAT SWIR X CO 2 and X CH 4 show similar features to those of the g-b FTS data except for the negative biases in the GOSAT data.

Description: Remote sensing of aerosols over snow using infrared AATSR observations Atmospheric Measurement Techniques, 4, 1133-1145, 2011 Author(s): L. G. Istomina, W. von Hoyningen-Huene, A. A. Kokhanovsky, E. Schultz, and J. P. Burrows Infrared (IR) retrievals of aerosol optical thickness (AOT) are challenging because of the low reflectance of aerosol layer at longer wavelengths. In this paper we present a closer analysis of this problem, performed with radiative transfer (RT) simulations for coarse and accumulation mode of four main aerosol components. It shows the strong angular dependence of aerosol IR reflectance at low solar elevations resulting from the significant asymmetry of aerosol phase function at these wavelengths. This results in detectable values of aerosol IR reflectance at certain non-nadir observation angles providing the advantage of multiangle remote sensing instruments for a retrieval of AOT at longer wavelengths. Such retrievals can be of importance e.g. in case of a very strong effect of the surface on the top of atmosphere (TOA) reflectance in the visible spectral range. In the current work, a new method to retrieve AOT of the coarse and accumulation mode particles over snow has been developed using the measurements of Advanced Along Track Scanning Radiometer (AATSR) on board the ENVISAT satellite. The algorithm uses AATSR channel at 3.7 μm and utilizes its dual-viewing observation technique, implying the forward view with an observation zenith angle of around 55 degrees and the nadir view. It includes cloud/snow discrimination, extraction of the atmospheric reflectance out of measured brightness temperature (BT) at 3.7 μm, and interpolation of look-up tables (LUTs) for a given aerosol reflectance. The algorithm uses LUTs, separately simulated with RT forward calculations. The resulting AOT at 500 nm is estimated from the value at 3.7 μm using a fixed Angström parameter. The presented method has been validated against ground-based Aerosol Robotic Network (AERONET) data for 4 high Arctic stations and shows good agreement. A case study has been performed at W-Greenland on 5 July 2008. The day before was characterized by a noticeable dust event. The retrieved AOT maps of the region show a clear increase of AOT in the Kangerlussuaq area. The area of increased AOT was detected on 5 July on the ice sheet east of Kangelussuaq, opposite to the observed north easterly wind at ground level. This position can be explained by a small scale atmospheric circulation transporting the mobilized mineral dust upslope, after its intrusion into the upper branch of the circulation. The performed study of atmospheric reflectance at 3.7 μm also shows possibilities for the detection and retrievals of cloud properties over snow surfaces.

Description: Analytical system for stable carbon isotope measurements of low molecular weight (C 2 -C 6 ) hydrocarbons Atmospheric Measurement Techniques, 4, 1161-1175, 2011 Author(s): A. Zuiderweg, R. Holzinger, and T. Röckmann We present setup, testing and initial results from a new automated system for stable carbon isotope ratio measurements on C 2 to C 6 atmospheric hydrocarbons. The inlet system allows analysis of trace gases from air samples ranging from a few liters for urban samples and samples with high mixing ratios, to many tens of liters for samples from remote unpolluted regions with very low mixing ratios. The centerpiece of the sample preparation is the separation trap, which is used to separate CO 2 and methane from the compounds of interest. The main features of the system are (i) the capability to sample up to 300 l of air, (ii) long term (since May 2009) operational δ 13 C accuracy levels in the range 0.3–0.8 ‰ (1-σ), and (iii) detection limits of order 1.5–2.5 ngC (collected amount of substance) for all reported compounds. The first application of this system was the analysis of 21 ambient air samples taken during 48 h in August 2009 in Utrecht, the Netherlands. Results obtained are generally in good agreement with those from similar urban ambient air studies. Short sample intervals allowed by the design of the instrument help to illustrate the complex diurnal behavior of hydrocarbons in an urban environment, where diverse sources, dynamical processes, and chemical reactions are present.

Description: Productivity response of calcareous nannoplankton in the South Atlantic to the Eocene Thermal Maximum 2 (ETM2) Climate of the Past Discussions, 7, 2089-2118, 2011 Author(s): M. Dedert, H. M. Stoll, D. Kroon, N. Shimizu, and P. Ziveri The Early Eocene Thermal Maximum 2 (ETM2) at ~53.7 Ma is one of multiple hyperthermal events that followed the Paleocene-Eocene Thermal Maximum (PETM, ~55 Ma). In order to reconstruct the primary productivity response to the ETM2 in the South Atlantic, we have analyzed Sr/Ca ratios in various size fractions of bulk sediments and in picked monogeneric populations of calcareous nannofossils. The latter technique of measuring selected nannofossil populations using the ion probe circumvents possible contamination with secondary calcite. Avoiding such contamination is important for interpretation of the nannoplankton productivity record, since diagenetic processes can bias the productivity signal, as we demonstrate for Sr/Ca measurements in the fine (

Description: Source brightness fluctuation correction of solar absorption fourier transform mid infrared spectra Atmospheric Measurement Techniques, 4, 1045-1051, 2011 Author(s): T. Ridder, T. Warneke, and J. Notholt The precision and accuracy of trace gas observations using solar absorption Fourier Transform infrared spectrometry depend on the stability of the light source. Fluctuations in the source brightness, however, cannot always be avoided. Current correction schemes, which calculate a corrected interferogram as the ratio of the raw DC interferogram and a smoothed DC interferogram, are applicable only to near infrared measurements. Spectra in the mid infrared spectral region below 2000 cm −1 are generally considered uncorrectable, if they are measured with a MCT detector. Such measurements introduce an unknown offset to MCT interferograms, which prevents the established source brightness fluctuation correction. This problem can be overcome by a determination of the offset using the modulation efficiency of the instrument. With known modulation efficiency the offset can be calculated, and the source brightness correction can be performed on the basis of offset-corrected interferograms. We present a source brightness fluctuation correction method which performs the smoothing of the raw DC interferogram in the interferogram domain by an application of a running mean instead of high-pass filtering the corresponding spectrum after Fourier transformation of the raw DC interferogram. This smoothing can be performed with the onboard software of commercial instruments. The improvement of MCT spectra and subsequent ozone profile and total column retrievals is demonstrated. Application to InSb interferograms in the near infrared spectral region proves the equivalence with the established correction scheme.

Description: Reconstruction of southeast Tibetan Plateau summer cloud cover over the past two centuries using tree ring δ 18 O Climate of the Past Discussions, 7, 1825-1844, 2011 Author(s): C. Shi, V. Daux, C. Risi, S.-G. Hou, M. Stievenard, M. Pierre, Z. Li, and V. Masson-Delmotte A tree-ring δ 18 O chronology of Linzhi spruce, spanning from AD 1781 to 2005, was developed in Bomi, Southeast Tibetan Plateau (TP). During the period with instrumental data (1961–2005), this record is strongly correlated with regional summer cloud cover, which is supported by a precipitation δ 18 O simulation conducted with the isotope-enabled atmospheric general circulation model LMDZiso. A 225-yr regional cloud cover reconstruction was therefore achieved. The observed cloud cover increased in the 1980s and this increase is not unprecedented in the entire reconstruction. The reconstructed cloud cover appears smaller and more stable in the 20th century than previously. A late 19th century decrease in our reconstructed cloud cover is consistent with a decrease in the TP glacier accumulation recorded in ice cores. Our data reveal a strong anomaly in the 1810s, which coincides with volcanic eruption in 1809 and the 1815 Tambora volcanic eruption.

Description: Volcanic and ENSO effects in China in simulations and reconstructions: Tambora eruption 1815 Climate of the Past Discussions, 7, 2061-2088, 2011 Author(s): D. Zhang, R. Blender, and K. Fraedrich The co-operative effects of volcanic eruptions and ENSO (El Niño/Southern Oscillation) on the climate in China are analyzed in a millennium simulation for 800–2005 AD using the earth system model (ESM) ECHAM5/MPIOM/JSBACH subject to anthropogenic and natural forcings. The experiment includes two ensembles with weak (5 members) and strong (3 members) total solar irradiance variability. In the absence of El Niño and La Niña events, volcanoes, which are the dominant forcing in both ensembles, cause a dramatic cooling in West China (−2 °C) and a drought in East China during the year after the eruption. The recovery times for the volcano induced cooling vary globally between one and 12 yr; in China these values are mostly within 1–4 yr, but reach 10 yr in the Northeast. Without volcanoes, after El Niño events the summer precipitation is reduced in the North, while South China becomes wetter (indicated by the Standardized Precipitation Index, SPI, for summers, JJA); La Niña events cause opposite effects. El Niño events in the winters after eruptions compensate the cooling in most regions of China, while La Niña events intensify the cooling (up to −2.5 °C). The simulated impact of the eruption of the Tambora in 1815, which caused the "year without summer" 1816 in Europe and North America and coldness and famines for several years in the Chinese province Yunnan, depends crucially on the ENSO state of the coupled model. A comparison with reconstructed El Niño events shows a moderate cool climate with wet (in the South) and extreme dry anomalies (in the North) persisting for several years.

Description: An improved NO 2 retrieval for the GOME-2 satellite instrument Atmospheric Measurement Techniques, 4, 1147-1159, 2011 Author(s): A. Richter, M. Begoin, A. Hilboll, and J. P. Burrows Satellite observations of nitrogen dioxide (NO 2 ) provide valuable information on both stratospheric and tropospheric composition. Nadir measurements from GOME, SCIAMACHY, OMI, and GOME-2 have been used in many studies on tropospheric NO 2 burdens, the importance of different NO x emissions sources and their change over time. The observations made by the three GOME-2 instruments will extend the existing data set by more than a decade, and a high quality of the data as well as their good consistency with existing time series is of particular importance. In this paper, an improved GOME-2 NO 2 retrieval is described which reduces the scatter of the individual NO 2 columns globally but in particular in the region of the Southern Atlantic Anomaly. This is achieved by using a larger fitting window including more spectral points, and by applying a two step spike removal algorithm in the fit. The new GOME-2 data set is shown to have good consistency with SCIAMACHY NO 2 columns. Remaining small differences are shown to be linked to changes in the daily solar irradiance measurements used in both GOME-2 and SCIAMACHY retrievals. In the large retrieval window, a not previously identified spectral signature was found which is linked to deserts and other regions with bare soil. Inclusion of this empirically derived pseudo cross-section significantly improves the retrievals and potentially provides information on surface properties and desert aerosols. Using the new GOME-2 NO 2 data set, a long-term average of tropospheric columns was computed and high-pass filtered. The resulting map shows evidence for pollution from several additional shipping lanes, not previously identified in satellite observations. This illustrates the excellent signal to noise ratio achievable with the improved GOME-2 retrievals.

Description: Matching radiative transfer models and radiosonde data from the EPS/Metop Sodankylä campaign to IASI measurements Atmospheric Measurement Techniques, 4, 1177-1189, 2011 Author(s): X. Calbet, R. Kivi, S. Tjemkes, F. Montagner, and R. Stuhlmann Radiances observed from IASI are compared to calculated ones. Calculated radiances are obtained using several radiative transfer models (OSS, LBLRTM v11.3 and v11.6) on best estimates of the atmospheric state vectors. The atmospheric state vectors are derived from cryogenic frost point hygrometer and humidity dry bias corrected RS92 measurements flown on sondes launched 1 h and 5 min before IASI overpass time. The temperature and humidity best estimate profiles are obtained by interpolating or extrapolating these measurements to IASI overpass time. The IASI observed and calculated radiances match to within one sigma IASI instrument noise in the spectral region where water vapour is a strong absorber (wavenumber, ν, in the range of 1500 ≤ ν ≤ 1570 and 1615 ≤ ν ≤ 1800 cm −1 ).

Description: Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes Atmospheric Measurement Techniques, 4, 1275-1289, 2011 Author(s): D. K. Farmer, J. R. Kimmel, G. Phillips, K. S. Docherty, D. R. Worsnop, D. Sueper, E. Nemitz, and J. L. Jimenez Although laboratory studies show that biogenic volatile organic compounds (VOCs) yield substantial secondary organic aerosol (SOA), production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR) PM 1 fluxes. Average deposition velocities for total NR-PM 1 aerosol at noon were 2.05 ± 0.04 mm s −1 . Using a high resolution measurement of the NH 2 + and NH 3 + fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s −1 and are dominated by deposition of ammonium sulphate.

Description: Space and ground segment performance and lessons learned of the FORMOSAT-3/COSMIC mission: four years in orbit Atmospheric Measurement Techniques, 4, 1115-1132, 2011 Author(s): C.-J. Fong, D. Whiteley, E. Yang, K. Cook, V. Chu, B. Schreiner, D. Ector, P. Wilczynski, T.-Y. Liu, and N. Yen The FORMOSAT-3/COSMIC (Constellation Observing System for Meteorology, Ionosphere, and Climate) Mission consisting of six Low-Earth-Orbit (LEO) satellites is the world's first demonstration constellation using radio occultation signals from Global Positioning System (GPS) satellites. The atmospheric profiles derived by processing radio occultation signals are retrieved in near real-time for global weather/climate monitoring, numerical weather prediction, and space weather research. The mission has processed, on average, 1400 to 1800 high-quality atmospheric sounding profiles per day. The atmospheric radio occultation data are assimilated into operational numerical weather prediction models for global weather prediction, including typhoon/hurricane/cyclone forecasts. The radio occultation data has shown a positive impact on weather predictions at many national weather forecast centers. A follow-on mission was proposed that transitions the current experimental research mission into a significantly improved real-time operational mission, which will reliably provide 8000 radio occultation soundings per day. The follow-on mission, as planned, will consist of 12 LEO satellites (compared to 6 satellites for the current mission) with data latency requirement of 45 min (compared to 3 h for the current mission), which will provide greatly enhanced opportunities for operational forecasts and scientific research. This paper will address the FORMOSAT-3/COSMIC system and mission overview, the spacecraft and ground system performance after four years in orbit, the lessons learned from the encountered technical challenges and observations, and the expected design improvements for the spacecraft and ground system for FORMOSAT-7/COSMIC-2.

Description: The Middle Miocene climate as modelled in an atmosphere-ocean-biosphere model Climate of the Past Discussions, 7, 1935-1972, 2011 Author(s): M. Krapp and J. H. Jungclaus We present simulations with a coupled ocean-atmosphere-biosphere model for the Middle Miocene 15 million years ago. The Middle Miocene topography, which alters both large-scale ocean and atmospheric circulations, causes a global warming of 0.7 K compared to present-day. Higher than present-day CO 2 levels of 480 and 720 ppm cause a global warming of 2.8 and 4.9 K, thereby matching proxy-based Middle Miocene global temperature estimates of 3–6 K warming. Higher CO 2 levels and the associated water vapour feedback enhance the greenhouse effect and lead to a polar amplification of the warming. Although oceanic and atmospheric poleward heat transport are individually altered by 10–30 % in the mid and high latitudes, changes of the total heat transport account only for 4–8 %, pointing toward a compensation between oceanic and atmospheric heat transport. Our model reproduces a denser vegetation in agreement with fossil records. These results suggest that higher than present-day CO 2 levels are essential to drive the warm Middle Miocene climate.

Description: Exploring Earth's atmosphere with radio occultation: contributions to weather, climate and space weather Atmospheric Measurement Techniques, 4, 1077-1103, 2011 Author(s): R. A. Anthes The launch of the proof-of-concept mission GPS/MET (Global Positioning System/Meteorology) in 1995 began a revolution in profiling Earth's atmosphere through radio occultation (RO). GPS/MET; subsequent single-satellite missions CHAMP (CHAllenging Minisatellite Payload), SAC-C (Satellite de Aplicaciones Cientificas-C), GRACE (Gravity Recovery and Climate Experiment), METOP-A, and TerraSAR-X (Beyerle et al., 2010); and the six-satellite constellation, FORMOSAT-3/COSMIC (Formosa Satellite mission {#}3/Constellation Observing System for Meteorology, Ionosphere, and Climate) have proven the theoretical capabilities of RO to provide accurate and precise profiles of electron density in the ionosphere and refractivity, containing information on temperature and water vapor, in the stratosphere and troposphere. This paper summarizes results from these RO missions and the applications of RO observations to atmospheric research and operational weather analysis and prediction.

Description: Synchronicity of the East Asian Summer Monsoon variability and Northern Hemisphere climate change since the last deglaciation Climate of the Past Discussions, 7, 2159-2192, 2011 Author(s): T. Shinozaki, M. Uchida, K. Minoura, M. Kondo, S. F. Rella, and Y. Shibata Understanding of the mechanism of the East Asian Summer Monsoon (EASM) is required for the prediction of climate change in East Asia in a scenario of modern global warming. In this study, we present high-resolution climate records from peat sediments in Northeast Japan to reconstruct the EASM variability based on peat bulk cellulose δ 13 C since the last deglaciation. We used a 8.8 m long peat sediment core collected from the Tashiro Bog, Northeast Japan. Based on 42 14 C measurements, the core bottom reaches ~15.5 ka. δ 13 C, accumulation rate and accumulation flux time-series correlate well to Greenland ice core δ 18 O variability, suggesting that the climate record in Northeast Japan is linked to global climate changes. The δ 13 C record at Tashiro Bog and other paleo-EASM records at Northeast and Southern China consistently demonstrate that hydrological environments were spatially different in mid-high and mid-low latitude regions over the last 15.5 kyr. During global cooling (warming) periods, mid-high and mid-low latitude regions were characterized by wet (dry) and dry (wet) environments, respectively. We suggest that these climatic patterns are related to the migration of the EASM-related rain belt during global climate changes, as a consequence of variations in intensity and location of both the Intertropical Convergence Zone (ITCZ) and the Western Pacific Subtropical High (STH). The location of the rain belt largely influences the East Asian hydrological environment. Our δ 13 C time-series are characterized by a 1230 yr throughout the Holocene and a 680 yr periodicity during the early Holocene. The 1230 yr periodicity is in agreement with North Atlantic ice-rafted debris (IRD) events, suggesting a teleconnection between the Northeast Japan and the North Atlantic during the Holocene. In addition, it is the first evidence that the Bond events were recorded in terrestrial sediment in Japan. On the other hand, the 680 yr periodicity between 10.0 and 8.0 kyr is consistent with a prominent 649 yr solar activity cycle, suggesting that solar activity affected EASM precipitation during the Hypsithermal, when orbital-scale solar insolation was at a maximum in the Northern Hemisphere.

Description: Detection of HO 2 by laser-induced fluorescence: calibration and interferences from RO 2 radicals Atmospheric Measurement Techniques, 4, 1209-1225, 2011 Author(s): H. Fuchs, B. Bohn, A. Hofzumahaus, F. Holland, K. D. Lu, S. Nehr, F. Rohrer, and A. Wahner HO 2 concentration measurements are widely accomplished by chemical conversion of HO 2 to OH including reaction with NO and subsequent detection of OH by laser-induced fluorescence. RO 2 radicals can be converted to OH via a similar radical reaction sequence including reaction with NO, so that they are potential interferences for HO 2 measurements. Here, the conversion efficiency of various RO 2 species to HO 2 is investigated. Experiments were conducted with a radical source that produces OH and HO 2 by water photolysis at 185 nm, which is frequently used for calibration of LIF instruments. The ratio of HO 2 and the sum of OH and HO 2 concentrations provided by the radical source was investigated and was found to be 0.50 ± 0.02. RO 2 radicals are produced by the reaction of various organic compounds with OH in the radical source. Interferences via chemical conversion from RO 2 radicals produced by the reaction of OH with methane and ethane (H-atom abstraction) are negligible consistent with measurements in the past. However, RO 2 radicals from OH plus alkene- and aromatic-precursors including isoprene (mainly OH-addition) are detected with a relative sensitivity larger than 80 % with respect to that for HO 2 for the configuration of the instrument with which it was operated during field campaigns. Also RO 2 from OH plus methyl vinyl ketone and methacrolein exhibit a relative detection sensitivity of 60 %. Thus, previous measurements of HO 2 radical concentrations with this instrument were biased in the presence of high RO 2 radical concentrations from isoprene, alkenes or aromatics, but were not affected by interferences in remote clean environment with no significant emissions of biogenic VOCs, when the OH reactivity was dominated by small alkanes. By reducing the NO concentration and/or the transport time between NO addition and OH detection, interference from these RO 2 species are suppressed to values below 20 % relative to the HO 2 detection sensitivity. The HO 2 conversion efficiency is also smaller by a factor of four, but this is still sufficient for atmospheric HO 2 concentration measurements for a wide range of conditions.

Description: Diode laser-based cavity ring-down instrument for NO 3 , N 2 O 5 , NO, NO 2 and O 3 from aircraft Atmospheric Measurement Techniques, 4, 1227-1240, 2011 Author(s): N. L. Wagner, W. P. Dubé, R. A. Washenfelder, C. J. Young, I. B. Pollack, T. B. Ryerson, and S. S. Brown This article presents a diode laser-based, cavity ring-down spectrometer for simultaneous in situ measurements of four nitrogen oxide species, NO 3 , N 2 O 5 , NO, NO 2 , as well as O 3 , designed for deployment on aircraft. The instrument measures NO 3 and NO 2 by optical extinction at 662 nm and 405 nm, respectively; N 2 O 5 is measured by thermal conversion to NO 3 , while NO and O 3 are measured by chemical conversion to NO 2 . The instrument has several advantages over previous instruments developed by our group for measurement of NO 2 , NO 3 and N 2 O 5 alone, based on a pulsed Nd:YAG and dye laser. First, the use of continuous wave diode lasers reduces the requirements for power and weight and eliminates hazardous materials. Second, detection of NO 2 at 405 nm is more sensitive than our previously reported 532 nm instrument, and does not have a measurable interference from O 3 . Third, the instrument includes chemical conversion of NO and O 3 to NO 2 to provide measurements of total NO x (= NO + NO 2 ) and O x (= NO 2 + O 3 ) on two separate channels; mixing ratios of NO and O 3 are determined by subtraction of NO 2 . Finally, all five species are calibrated against a single standard based on 254 nm O 3 absorption to provide high accuracy. Disadvantages include an increased sensitivity to water vapor on the 662 nm NO 3 and N 2 O 5 channels and a modest reduction in sensitivity for these species compared to the pulsed laser instrument. The in-flight detection limit for both NO 3 and N 2 O 5 is 3 pptv (2 σ, 1 s) and for NO, NO 2 and O 3 is 140, 90, and 120 pptv (2 σ, 1 s) respectively. Demonstrated performance of the instrument in a laboratory/ground based environment is better by approximately a factor of 2–3. The NO and NO 2 measurements are less precise than research-grade chemiluminescence instruments. However, the combination of these five species in a single instrument, calibrated to a single analytical standard, provides a complete and accurate picture of nighttime nitrogen oxide chemistry. The instrument performance is demonstrated using data acquired during a recent field campaign in California.

Description: Retrieval of water vapor vertical distributions in the upper troposphere and the lower stratosphere from SCIAMACHY limb measurements Atmospheric Measurement Techniques, 4, 933-954, 2011 Author(s): A. Rozanov, K. Weigel, H. Bovensmann, S. Dhomse, K.-U. Eichmann, R. Kivi, V. Rozanov, H. Vömel, M. Weber, and J. P. Burrows This study describes the retrieval of water vapor vertical distributions in the upper troposphere and lower stratosphere (UTLS) altitude range from space-borne observations of the scattered solar light made in limb viewing geometry. First results using measurements from SCIAMACHY (Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY) aboard ENVISAT (Environmental Satellite) are presented here. In previous publications, the retrieval of water vapor vertical distributions has been achieved exploiting either the emitted radiance leaving the atmosphere or the transmitted solar radiation. In this study, the scattered solar radiation is used as a new source of information on the water vapor content in the UTLS region. A recently developed retrieval algorithm utilizes the differential absorption structure of the water vapor in 1353–1410 nm spectral range and yields the water vapor content in the 11–25 km altitude range. In this study, the retrieval algorithm is successfully applied to SCIAMACHY limb measurements and the resulting water vapor profiles are compared to in situ balloon-borne observations. The results from both satellite and balloon-borne instruments are found to agree typically within 10 %.

Description: Sensitivity of interglacial Greenland temperature and δ 18 O to orbital and CO 2 forcing: climate simulations and ice core data Climate of the Past Discussions, 7, 1585-1630, 2011 Author(s): V. Masson-Delmotte, P. Braconnot, G. Hoffmann, J. Jouzel, M. Kageyama, A. Landais, Q. Lejeune, C. Risi, L. Sime, J. Sjolte, D. Swingedouw, and B. Vinther The sensitivity of interglacial Greenland temperature to orbital and CO 2 forcing is investigated using the NorthGRIP ice core data and coupled ocean-atmosphere IPSL-CM4 model simulations. These simulations were conducted in response to different interglacial orbital configurations, and to increased CO 2 concentrations. These different forcings cause very distinct simulated seasonal and latitudinal temperature and water cycle changes, limiting the analogies between the last interglacial and future climate. However, the IPSL-CM4 model shows similar magnitudes of Arctic summer warming and climate feedbacks in response to 2 × CO 2 and orbital forcing of the last interglacial period (126 000 yr ago). The IPSL model produces a remarkably linear relationship between top of atmosphere incoming summer solar radiation and simulated changes in summer and annual mean central Greenland temperature. This contrasts with the stable isotope record from the Greenland ice cores, showing a multi-millennial lagged response to summer insolation. During the early part of interglacials, the observed lags may be explained by ice sheet-ocean feedbacks linked with changes in ice sheet elevation and the impact of meltwater on ocean circulation, as investigated with sensitivity studies. A quantitative comparison between ice core data and climate simulations requires to explore the stability of the stable isotope – temperature relationship. Atmospheric simulations including water stable isotopes have been conducted with the LMDZiso model under different boundary conditions. This set of simulations allows to calculate a temporal Greenland isotope-temperature slope (0.3–0.4 ‰ per °C) during warmer than present Arctic climates, in response to increased CO 2 , increased ocean temperature and orbital forcing. This temporal slope appears twice as small as the modern spatial gradient and is consistent with other ice core estimates. A preliminary comparison with other model results implies that other mechanisms could also play a role. This suggests that further simulations and detailed inter-model comparisons are also likely to be of benefit. Comparisons with Greenland ice core stable isotope data reveals that IPSL/LMDZiso simulations strongly underestimate the amplitude of the ice core signal during the last interglacial, which could reach +8–10 °C at fixed-elevation. While the model-data mismatch may result from missing positive feedbacks (e.g. vegetation), it could also be explained by a reduced elevation of the central Greenland ice sheet surface by 300–400 m.

Description: Fast NO 2 retrievals from Odin-OSIRIS limb scatter measurements Atmospheric Measurement Techniques, 4, 965-972, 2011 Author(s): A. E. Bourassa, C. A. McLinden, C. E. Sioris, S. Brohede, A. F. Bathgate, E. J. Llewellyn, and D. A. Degenstein The feasibility of retrieving vertical profiles of NO 2 from space-based measurements of limb scattered sunlight has been demonstrated using several different data sets since the 1980's. The NO 2 data product routinely retrieved from measurements made by the Optical Spectrograph and InfraRed Imaging System (OSIRIS) instrument onboard the Odin satellite uses a spectral fitting technique over the 437 to 451 nm range, over which there are 36 individual wavelength measurements. In this work we present a proof of concept technique for the retrieval of NO 2 using only 4 of the 36 OSIRIS measurements in this wavelength range, which reduces the computational cost by almost an order of magnitude. The method is an adaptation of a triplet analysis technique that is currently used for the OSIRIS retrievals of ozone at Chappuis band wavelengths. The results obtained are shown to be in very good agreement with the spectral fit method, and provide an important alternative for applications where the computational burden is very high. Additionally this provides a baseline for future instrument design in terms of cost effectiveness and reducing spectral range requirements.

Description: Intercomparison of stratospheric gravity wave observations with AIRS and IASI Atmospheric Measurement Techniques, 7, 4517-4537, 2014 Author(s): L. Hoffmann, M. J. Alexander, C. Clerbaux, A. W. Grimsdell, C. I. Meyer, T. Rößler, and B. Tournier Gravity waves are an important driver for the atmospheric circulation and have substantial impact on weather and climate. Satellite instruments offer excellent opportunities to study gravity waves on a global scale. This study focuses on observations from the Atmospheric Infrared Sounder (AIRS) onboard the National Aeronautics and Space Administration Aqua satellite and the Infrared Atmospheric Sounding Interferometer (IASI) onboard the European MetOp satellites. The main aim of this study is an intercomparison of stratospheric gravity wave observations of both instruments. In particular, we analyzed AIRS and IASI 4.3 μm brightness temperature measurements, which directly relate to stratospheric temperature. Three case studies showed that AIRS and IASI provide a clear and consistent picture of the temporal development of individual gravity wave events. Statistical comparisons based on a 5-year period of measurements (2008–2012) showed similar spatial and temporal patterns of gravity wave activity. However, the statistical comparisons also revealed systematic differences of variances between AIRS and IASI that we attribute to the different spatial measurement characteristics of both instruments. We also found differences between day- and nighttime data that are partly due to the local time variations of the gravity wave sources. While AIRS has been used successfully in many previous gravity wave studies, IASI data are applied here for the first time for that purpose. Our study shows that gravity wave observations from different hyperspectral infrared sounders such as AIRS and IASI can be directly related to each other, if instrument-specific characteristics such as different noise levels and spatial resolution and sampling are carefully considered. The ability to combine observations from different satellites provides an opportunity to create a long-term record, which is an exciting prospect for future climatological studies of stratospheric gravity wave activity.

Description: Collection efficiency of the soot-particle aerosol mass spectrometer (SP-AMS) for internally mixed particulate black carbon Atmospheric Measurement Techniques, 7, 4507-4516, 2014 Author(s): M. D. Willis, A. K. Y. Lee, T. B. Onasch, E. C. Fortner, L. R. Williams, A. T. Lambe, D. R. Worsnop, and J. P. D. Abbatt The soot-particle aerosol mass spectrometer (SP-AMS) uses an intra-cavity infrared laser to vaporize refractory black carbon (rBC) containing particles, making the particle beam–laser beam overlap critical in determining the collection efficiency (CE) for rBC and associated non-refractory particulate matter (NR-PM). This work evaluates the ability of the SP-AMS to quantify rBC and NR-PM mass in internally mixed particles with different thicknesses of organic coating. Using apparent relative ionization efficiencies for uncoated and thickly coated rBC particles, we report measurements of SP-AMS sensitivity to NR-PM and rBC, for Regal Black, the recommended particulate calibration material. Beam width probe (BWP) measurements are used to illustrate an increase in sensitivity for highly coated particles due to narrowing of the particle beam, which enhances the CE of the SP-AMS by increasing the laser beam–particle beam overlap. Assuming complete overlap for thick coatings, we estimate CE for bare Regal Black particles of 0.6 ± 0.1, which suggests that previously measured SP-AMS sensitivities to Regal Black were underestimated by up to a factor of 2. The efficacy of the BWP measurements is highlighted by studies at a busy road in downtown Toronto and at a non-roadside location, which show particle beam widths similar to, but greater than that of bare Regal Black and coated Regal Black, respectively. Further BWP measurements at field locations will help to constrain the range of CE for fresh and aged rBC-containing particles. The ability of the SP-AMS to quantitatively assess the composition of internally mixed particles is validated through measurements of laboratory-generated organic coated particles, which demonstrate that the SP-AMS can quantify rBC and NR-PM over a wide range of particle compositions and rBC core sizes.

Description: Reference quality upper-air measurements: GRUAN data processing for the Vaisala RS92 radiosonde Atmospheric Measurement Techniques, 7, 4463-4490, 2014 Author(s): R. J. Dirksen, M. Sommer, F. J. Immler, D. F. Hurst, R. Kivi, and H. Vömel The GCOS (Global Climate Observing System) Reference Upper-Air Network (GRUAN) data processing for the Vaisala RS92 radiosonde was developed to meet the criteria for reference measurements. These criteria stipulate the collection of metadata, the use of well-documented correction algorithms, and estimates of the measurement uncertainty. An important and novel aspect of the GRUAN processing is that the uncertainty estimates are vertically resolved. This paper describes the algorithms that are applied in version 2 of the GRUAN processing to correct for systematic errors in radiosonde measurements of pressure, temperature, humidity, and wind, as well as how the uncertainties related to these error sources are derived. Currently, the RS92 is launched on a regular basis at 13 out of 15 GRUAN sites. An additional GRUAN requirement for performing reference measurements with the RS92 is that the manufacturer-prescribed procedure for the radiosonde's preparation, i.e. heated reconditioning of the sensors and recalibration during ground check, is followed. In the GRUAN processing however, the recalibration of the humidity sensors that is applied during ground check is removed. For the dominant error source, solar radiation, laboratory experiments were performed to investigate and model its effect on the RS92's temperature and humidity measurements. GRUAN uncertainty estimates are 0.15 K for night-time temperature measurements and approximately 0.6 K at 25 km during daytime. The other uncertainty estimates are up to 6% relative humidity for humidity, 10–50 m for geopotential height, 0.6 hPa for pressure, 0.4–1 m s −1 for wind speed, and 1° for wind direction. Daytime temperature profiles for GRUAN and Vaisala processing are comparable and consistent within the estimated uncertainty. GRUAN daytime humidity profiles are up to 15% moister than Vaisala processed profiles, of which two-thirds is due to the radiation dry bias correction and one-third is due to an additional calibration correction. Redundant measurements with frost point hygrometers (CFH and NOAA FPH) show that GRUAN-processed RS92 humidity profiles and frost point data agree within 15% in the troposphere. No systematic biases occur, apart from a 5% dry bias for GRUAN data around −40 °C at night.

Description: Deployment of a sequential two-photon laser-induced fluorescence sensor for the detection of gaseous elemental mercury at ambient levels: fast, specific, ultrasensitive detection with parts-per-quadrillion sensitivity Atmospheric Measurement Techniques, 7, 4251-4265, 2014 Author(s): D. Bauer, S. Everhart, J. Remeika, C. Tatum Ernest, and A. J. Hynes The operation of a laser-based sensor for gas-phase elemental mercury, Hg(0), is described. It utilizes sequential two-photon laser excitation with detection of blue-shifted laser-induced fluorescence (LIF) to provide a highly specific detection scheme that precludes detection of anything other than atomic mercury. It has high sensitivity, fast temporal resolution, and can be deployed for in situ measurements in the open atmosphere with essentially no perturbation of the environment. An ambient sample can also be pulled through a fluorescence cell, allowing for standard addition calibrations of the concentration. No type of preconcentration is required and there appears to be no significant interferences from other atmospheric constituents, including gas-phase oxidized mercury species. As a consequence, it is not necessary to remove oxidized mercury, commonly referred to as reactive gaseous mercury (RGM), from the air sample. The instrument has been deployed as part of an instrument intercomparison and compares well with conventional instrumentation that utilizes preconcentration on gold followed by analysis using cold-vapor atomic fluorescence spectroscopy (CVAFS). Currently, the achievable detection sensitivity is ~ 15 pg m −3 (~ 5 × 10 4 atoms cm −3 , ~ 2 ppq) at a sampling rate of 0.1 Hz, i.e., averaging 100 shots with a 10 Hz laser system. Preliminary results are described for a 50 Hz instrument that utilizes a modified excitation sequence and has monitored ambient elemental mercury with an effective sampling rate of 10 Hz. Additional work is required to produce the precision necessary to perform eddy correlation measurements. Addition of a pyrolysis channel should allow for the measurement of total gaseous mercury (TGM) and hence RGM (by difference) with good sensitivity and time resolution.

Description: Prerequisites for application of hyperbolic relaxed eddy accumulation on managed grasslands and alternative net ecosystem exchange flux partitioning Atmospheric Measurement Techniques, 7, 4237-4250, 2014 Author(s): M. Riederer, J. Hübner, J. Ruppert, W. A. Brand, and T. Foken Relaxed eddy accumulation is still applied in ecosystem sciences for measuring trace gas fluxes. On managed grasslands, the length of time between management events and the application of relaxed eddy accumulation has an essential influence on the determination of the proportionality factor b and thus on the resulting flux. In this study this effect is discussed for the first time. Also, scalar similarity between proxy scalars and scalars of interest is affected until the ecosystem has completely recovered. Against this background, CO 2 fluxes were continuously measured and 13 CO 2 isofluxes were determined with a high measurement precision on two representative days in summer 2010. Moreover, a common method for the partitioning of the net ecosystem exchange into assimilation and respiration based on temperature and light response was compared with an isotopic approach directly based on the isotope discrimination of the biosphere. This approach worked well on the grassland site and could enhance flux partitioning results by better reproducing the environmental conditions.

Description: Extending the satellite data record of tropospheric ozone profiles from Aura-TES to MetOp-IASI: characterisation of optimal estimation retrievals Atmospheric Measurement Techniques, 7, 4223-4236, 2014 Author(s): H. Oetjen, V. H. Payne, S. S. Kulawik, A. Eldering, J. Worden, D. P. Edwards, G. L. Francis, H. M. Worden, C. Clerbaux, J. Hadji-Lazaro, and D. Hurtmans We apply the Tropospheric Emission Spectrometer (TES) ozone retrieval algorithm to Infrared Atmospheric Sounding Instrument (IASI) radiances and characterise the uncertainties and information content of the retrieved ozone profiles. This study focuses on mid-latitudes for the year 2008. We validate our results by comparing the IASI ozone profiles to ozone sondes. In the sonde comparisons, we find a negative bias (1–10%) in the IASI profiles in the lower to mid-troposphere and a positive bias (up to 14%) in the upper troposphere/lower stratosphere (UTLS) region. For the described cases, the degrees of freedom for signal are on average 3.2, 0.3, 0.8, and 0.9 for the columns 0 km – top of atmosphere, (0–6), (0–11), and (8–16) km, respectively. We find that our biases with respect to sondes and our degrees of freedom for signal for ozone are comparable to previously published results from other IASI ozone algorithms. In addition to evaluating biases, we validate the retrieval errors by comparing predicted errors to the sample covariance matrix of the IASI observations themselves. For the predicted versus empirical error comparison, we find that these errors are consistent and that the measurement noise and the interference of temperature and water vapour on the retrieval together mostly explain the empirically derived random errors. In general, the precision of the IASI ozone profiles is better than 20%.

Description: Solar irradiances measured using SPN1 radiometers: uncertainties and clues for development Atmospheric Measurement Techniques, 7, 4267-4283, 2014 Author(s): J. Badosa, J. Wood, P. Blanc, C. N. Long, L. Vuilleumier, D. Demengel, and M. Haeffelin The fast development of solar radiation and energy applications, such as photovoltaic and solar thermodynamic systems, has increased the need for solar radiation measurement and monitoring, for not only the global but also the diffuse and direct components. End users look for the best compromise between getting close to state-of-the-art measurements and keeping low capital, maintenance and operating costs. Among the existing commercial options, SPN1 is a relatively low cost solar radiometer that estimates global and diffuse solar irradiances from seven thermopile sensors under a shading mask and without moving parts. This work presents a comprehensive study of SPN1 accuracy and sources of uncertainty, drawing on laboratory experiments, numerical modelling and comparison studies between measurements from this sensor and state-of-the art instruments for six diverse sites. Several clues are provided for improving the SPN1 accuracy and agreement with state-of-the art measurements.

Description: Differences in aerosol absorption Ångström exponents between correction algorithms for a particle soot absorption photometer measured on the South African Highveld Atmospheric Measurement Techniques, 7, 4285-4298, 2014 Author(s): J. Backman, A. Virkkula, V. Vakkari, J. P. Beukes, P. G. Van Zyl, M. Josipovic, S. Piketh, P. Tiitta, K. Chiloane, T. Petäjä, M. Kulmala, and L. Laakso Absorption Ångström exponents (AAEs) calculated from filter-based absorption measurements are often used to give information on the origin of the ambient aerosol, for example, to distinguish between urban pollution and biomass burning aerosol. Filter-based absorption measurements are widely used and are common at aerosol monitoring stations globally. Several correction algorithms are used to account for artefacts associated with filter-based absorption techniques. These algorithms are of profound importance when determining the absolute amount of absorption by the aerosol. However, this study shows that there are substantial differences between the AAEs calculated from these corrections. Depending on the used correction, AAEs can change by as much as 46%. The study also highlights that the difference between AAEs calculated using different corrections can lead to conflicting conclusions on the type of aerosol when using the same data set. The AAE ranged between 1.17 for non-corrected data to 1.96 for the correction that gave the greatest values. Furthermore, the study implies that the AAEs reported for a site depend on at which filter transmittance the filter is changed. In this work, the AAEs were calculated from data measured with a three-wavelength particle soot absorption photometer (PSAP) at Elandsfontein on the South African Highveld for 23 months. The sample air of the PSAP was diluted to prolong filter change intervals, by a factor of 15. The correlation coefficient between the dilution-corrected PSAP and a non-diluted Multi-Angle Absorption Photometer (MAAP) was 0.9. Thus, the study also shows that the applicability of the PSAP can be extended to remote sites that are not often visited or suffer from high levels of pollution.

Description: Looking through the haze: evaluating the CALIPSO level 2 aerosol optical depth using airborne high spectral resolution lidar data Atmospheric Measurement Techniques, 7, 4317-4340, 2014 Author(s): R. R. Rogers, M. A. Vaughan, C. A. Hostetler, S. P. Burton, R. A. Ferrare, S. A. Young, J. W. Hair, M. D. Obland, D. B. Harper, A. L. Cook, and D. M. Winker The Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument onboard the Cloud–Aerosol Lidar and Pathfinder Satellite Observations (CALIPSO) spacecraft has provided over 8 yr of nearly continuous vertical profiling of Earth's atmosphere. In this paper we investigate the V3.01 and V3.02 CALIOP 532 nm aerosol layer optical depth (AOD) product (i.e the AOD of individual layers) and the column AOD product (i.e., the sum AOD of the complete column) using an extensive database of coincident measurements. The CALIOP AOD measurements and AOD uncertainty estimates are compared with collocated AOD measurements collected with the NASA High Spectral Resolution Lidar (HSRL) in the North American and Caribbean regions. In addition, the CALIOP aerosol lidar ratios are investigated using the HSRL measurements. In general, compared with the HSRL values, the CALIOP layer AOD are biased high by less than 50% for AOD 〈 0.3 with higher errors for higher AOD. Less than 60% of the HSRL AOD measurements are encompassed within the CALIOP layer 1 SD uncertainty range (around the CALIOP layer AOD), so an error estimate is created to encompass 68% of the HSRL data. Using this new metric, the CALIOP layer AOD error is estimated using the HSRL layer AOD as ±0.035 ± 0.05 · (HSRL layer AOD) at night and ±0.05 ± 0.05 · (HSRL layer AOD) during the daytime. Furthermore, the CALIOP layer AOD error is found to correlate with aerosol loading as well as aerosol subtype, with the AODs in marine and dust layers agreeing most closely with the HSRL values. The lidar ratios used by CALIOP for polluted dust, polluted continental, and biomass burning layers are larger than the values measured by the HSRL in the CALIOP layers, and therefore the AODs for these types retrieved by CALIOP were generally too large. We estimated the CALIOP column AOD error can be expressed as ±0.05 ± 0.07 · (HSRL column AOD) at night and ±0.08 ± 0.1 · (HSRL column AOD) during the daytime. Multiple sources of error contribute to both positive and negative errors in the CALIOP column AOD, including multiple layers in the column of different aerosol types, lidar ratio errors, cloud misclassification, and undetected aerosol layers. The undetected layers were further investigated and we found that the layer detection algorithm works well at night, although undetected aerosols in the free troposphere introduce a mean underestimate of 0.02 in the column AOD in the data set examined. The decreased signal-to-noise ratio (SNR) during the daytime led to poorer performance of the layer detection. This caused the daytime CALIOP column AOD to be less accurate than during the nighttime, because CALIOP frequently does not detect optically thin aerosol layers with AOD 〈 0.1. Given that the median vertical extent of aerosol detected within any column was 1.6 km during the nighttime and 1.5 km during the daytime, we can estimate the minimum extinction detection threshold to be 0.012 km −1 at night and 0.067 km −1 during the daytime in a layer median sense. This extensive validation of level 2 CALIOP AOD products extends previous validation studies to nighttime lighting conditions and provides independent measurements of the lidar ratio; thus, allowing the assessment of the effect on the CALIOP AOD of using inappropriate lidar ratio values in the extinction retrieval.

Description: The use of NO 2 absorption cross section temperature sensitivity to derive NO 2 profile temperature and stratospheric–tropospheric column partitioning from visible direct-sun DOAS measurements Atmospheric Measurement Techniques, 7, 4299-4316, 2014 Author(s): E. Spinei, A. Cede, W. H. Swartz, J. Herman, and G. H. Mount This paper presents a temperature sensitivity method (TESEM) to accurately calculate total vertical NO 2 column, atmospheric slant NO 2 profile-weighted temperature ( T ), and to separate stratospheric and tropospheric columns from direct-sun (DS), ground-based measurements using the retrieved T . TESEM is based on differential optical absorption spectroscopy (DOAS) fitting of the linear temperature-dependent NO 2 absorption cross section, σ ( T ), regression model (Vandaele et al., 2003). Separation between stratospheric and tropospheric columns is based on the primarily bimodal vertical distribution of NO 2 and an assumption that stratospheric effective temperature can be represented by temperature at 27 km ± 3 K, and tropospheric effective temperature is equal to surface temperature within 3–5 K. These assumptions were derived from the Global Modeling Initiative (GMI) chemistry-transport model (CTM) simulations over two northern midlatitude sites in 2011. TESEM was applied to the Washington State University Multi-Function DOAS instrument (MFDOAS) measurements at four midlatitude locations with low and moderate NO 2 anthropogenic emissions: (1) the Jet Propulsion Laboratory's Table Mountain Facility (JPL-TMF), CA, USA (34.38° N/117.68° W); (2) Pullman, WA, USA (46.73° N/117.17° W); (3) Greenbelt, MD, USA (38.99° N/76.84° W); and (4) Cabauw, the Netherlands (51.97° N/4.93° E) during July 2007, June–July 2009, July–August and October 2011, November 2012–May 2013, respectively. NO 2 T and total, stratospheric, and tropospheric NO 2 vertical columns were determined over each site.

Description: A Fabry–Perot interferometer-based camera for two-dimensional mapping of SO 2 distributions Atmospheric Measurement Techniques, 7, 3705-3715, 2014 Author(s): J. Kuhn, N. Bobrowski, P. Lübcke, L. Vogel, and U. Platt We examine a new imaging method for the remote sensing of volcanic gases, which relies on the regularly spaced narrow-band absorption structures in the UV–VIS of many molecules. A Fabry–Perot interferometer (FPI) is used to compare the scattered sunlight radiance at wavelengths corresponding to absorption bands with the radiance at wavelengths in between the bands, thereby identifying and quantifying the gas. In this first theoretical study, we present sample calculations for the detection of sulfur dioxide (SO 2 ). Optimum values for the FPI setup parameters are proposed. Furthermore, the performance of the FPI method is compared to SO 2 cameras. We show that camera systems using an FPI are far less influenced by changes in atmospheric radiative transfer (e.g., due to aerosol) and have a great potential as a future technique for examining emissions of SO 2 (or other gases) from volcanic sources and other point sources.

Description: Middle-atmospheric zonal and meridional wind profiles from polar, tropical and midlatitudes with the ground-based microwave Doppler wind radiometer WIRA Atmospheric Measurement Techniques, 7, 4491-4505, 2014 Author(s): R. Rüfenacht, A. Murk, N. Kämpfer, P. Eriksson, and S. A. Buehler WIRA is a ground-based microwave Doppler spectroradiometer specifically designed for the measurement of profiles of horizontal wind in the upper stratosphere and lower mesosphere region where no other continuously running measurement technique exists. A proof of principle has been delivered in a previous publication. A technical upgrade including a new high-frequency amplifier and sideband filter has improved the signal to noise ratio by a factor of 2.4. Since this upgrade the full horizontal wind field comprising zonal and meridional wind profiles is continuously measured. A completely new retrieval based on optimal estimation has been set up. Its characteristics are detailed in the present paper. Since the start of the routine operation of the first prototype in September 2010, WIRA has been measuring at four different locations at polar, mid- and tropical latitudes (67°22' N/26°38' E, 46°57' N/7°26' E, 43°56' N/5°43' E and 21°04' S/55°23' E) for time periods between 5.5 and 11 months. The data presented in this paper are daily average wind profiles with typical uncertainties and resolutions of 10 to 20 m s −1 and 10 to 16 km, respectively. A comparison between the data series from WIRA and European Centre for Medium-Range Weather Forecasts (ECMWF) model data revealed agreement within 10% in the stratospheric zonal wind. The meridional wind profiles agree within their error bars over the entire sensitive altitude range of WIRA. However, significant differences in the mesospheric zonal wind speed of up to 50% have been found.

Description: The sharp decline of East Asian summer monsoon at mid-Holocene indicated by the lake-wetland transition in the Sanjiang Plain, northeastern China Climate of the Past Discussions, 10, 4595-4622, 2014 Author(s): Z. Q. Zhang, G. P. Wang, X. G. Lv, H. J. Jia, and Q. H. Xu The timing of the waxing and wining of the East Asian summer monsoon during the Holocene is still under debate. In present study, we present the high-resolution grain-size and LOI records from a well-dated mud/peat profile to reveal the lake-wetland transition in the Sanjiang Plain and discuss its significance to Holocene monsoon evolutions. The results show that the shallow-water lakes have developed in low-lying areas of the plain before 4600 yr BP, corresponding to the Holocene monsoon maximum. Thereafter, the wetlands began to initiate with the extinction of the paleolakes, marking a lake-shrinking stage with the relative dry climate. Considering the prevalent monsoon climate in the Sanjiang Plain, we suggest the lake-wetland transition at 4600 yr BP indicate a sharp decline of the summer monsoon rather than the basin infilling process. Such a remarkable monsoon weakening event has been widely documented in northern China, and we associated it with the ocean–atmosphere interacting processes in low-latitude regions.

Description: A two thousand year annual record of snow accumulation rates for Law Dome, East Antarctica Climate of the Past Discussions, 10, 4469-4497, 2014 Author(s): J. Roberts, C. Plummer, T. Vance, T. van Ommen, A. Moy, S. Poynter, A. Treverrow, M. Curran, and S. George Accurate high resolution records of snow accumulation rates in Antarctica are crucial for estimating ice sheet mass balance and subsequent sea level change. Snowfall rates at Law Dome, East Antarctica, have been linked with regional atmospheric circulation to mid-latitudes as well as regional Antarctic snowfall. Here, we extend the Law Dome accumulation record from 750 to 2035 years, using recent annual layer dating that extends to AD −22. Accumulation rates were calculated as the ratio of measured to modelled layer thicknesses, multiplied by the long term mean accumulation rate. The modelled layer thicknesses were based on a power law vertical strain rate profile fitted to observed annual layer thickness. The periods AD 380–442, AD 727–783 and AD 1970–2009 have above average snow accumulation rates, while AD 663–704, AD 933–975 and AD 1429–1468 were below average. The calculated snow accumulation rates show good correlation with atmospheric reanalysis estimates, and significant spatial correlation over a wide expanse of East Antarctica, demonstrating that the Law Dome record captures larger scale variability across a large region of East Antarctica well beyond the immediate vicinity of the Law Dome summit. Spectral analysis reveals periodicities in the snow accumulation record which may be related to ENSO and Interdecadal Pacific Oscillation frequencies.

Description: Analysis of internal gravity waves with GPS RO density profiles Atmospheric Measurement Techniques, 7, 4123-4132, 2014 Author(s): P. Šácha, U. Foelsche, and P. Pišoft GPS radio occultation (RO) data have proved to be a great tool for atmospheric monitoring and studies. In the past decade, they were frequently used for analyses of the internal gravity waves in the upper troposphere and lower stratosphere region. Atmospheric density is the first quantity of state gained in the retrieval process and is not burdened by additional assumptions. However, there are no studies elaborating in detail the utilization of GPS RO density profiles for gravity wave analyses. In this paper, we introduce a method for density background separation and a methodology for internal gravity wave analysis using the density profiles. Various background choices are discussed and the correspondence between analytical forms of the density and temperature background profiles is examined. In the stratosphere, a comparison between the power spectrum of normalized density and normalized dry temperature fluctuations confirms the suitability of the density profiles' utilization. In the height range of 8–40 km, results of the continuous wavelet transform are presented and discussed. Finally, the limits of our approach are discussed and the advantages of the density usage are listed.

Description: Characterization of model errors in the calculation of tangent heights for atmospheric infrared limb measurements Atmospheric Measurement Techniques, 7, 4117-4122, 2014 Author(s): M. Ridolfi and L. Sgheri We review the main factors driving the calculation of the tangent height of spaceborne limb measurements: the ray-tracing method, the refractive index model and the assumed atmosphere. We find that commonly used ray tracing and refraction models are very accurate, at least in the mid-infrared. The factor with largest effect in the tangent height calculation is the assumed atmosphere. Using a climatological model in place of the real atmosphere may cause tangent height errors up to ± 200 m. Depending on the adopted retrieval scheme, these errors may have a significant impact on the derived profiles.

Description: Recovering long-term aerosol optical depth series (1976–2012) from an astronomical potassium-based resonance scattering spectrometer Atmospheric Measurement Techniques, 7, 4103-4116, 2014 Author(s): A. Barreto, E. Cuevas, P. Pallé, P. M. Romero, C. Guirado, C. J. Wehrli, and F. Almansa A 37-year long-term series of monochromatic aerosol optical depth (AOD) has been recovered from solar irradiance measurements performed with the solar spectrometer Mark-I, deployed at Izaña mountain since 1976. The instrument operation is based on the method of resonant scattering, which affords wavelength absolute reference and stability (long-term stability and high precision) in comparison to other instruments based purely on interference filters. However, it has been specifically designed as a reference instrument for helioseismology, and its ability to determine AOD from transmitted and scattered monochromatic radiation at 769.9 nm inside a potassium vapour cell in the presence of a permanent magnetic field is evaluated in this paper. Particularly, the use of an exposed mirror arrangement to collect sunlight as well as the Sun–laboratory velocity dependence of the scattered component introduces some important inconveniences to overcome when we perform the instrument's calibration. We have solved this problem using a quasi-continuous Langley calibration technique and a refinement procedure to correct for calibration errors as well as for the fictitious diurnal cycle on AOD data. Our results showed similar calibration errors retrieved by means of this quasi-continuous Langley technique applied in different aerosol load events (from 0.04 to 0.3), provided aerosol concentration remains constant throughout the calibration interval. It assures the validity of this technique when it is applied in those periods with relatively high aerosol content. The comparative analysis between the recovered AOD data set from the Mark-I and collocated quasi-simultaneous data from the Cimel-AErosol RObotic NETwork (AERONET) and Precision Filter Radiometer (PFR) instruments showed an absolute mean bias ≤ 0.01 in the 10- and 12-year comparison, respectively. High correlation coefficients between AERONET and Mark-I and PFR/Mark-I pairs confirmed a very good linear relationship between instruments, proving that recovered AOD data series from Mark-I can be used together with PFR and AERONET AOD data to build a long-term AOD data series at the Izaña site (1976–now), suitable for future analysis of aerosols trends and inter-annual variability. Finally, the AOD preliminary trend analysis in the 29-year period from 1984 to 2012 with Mark-I AOD revealed no significant trends.

Description: Multistation intercomparison of column-averaged methane from NDACC and TCCON: impact of dynamical variability Atmospheric Measurement Techniques, 7, 4081-4101, 2014 Author(s): A. Ostler, R. Sussmann, M. Rettinger, N. M. Deutscher, S. Dohe, F. Hase, N. Jones, M. Palm, and B.-M. Sinnhuber Dry-air column-averaged mole fractions of methane (XCH 4 ) retrieved from ground-based solar Fourier transform infrared (FTIR) measurements provide valuable information for satellite validation, evaluation of chemical-transport models, and source-sink-inversions. In this context, Sussmann et al. (2013) have shown that midinfrared (MIR) soundings from the Network for the Detection of Atmospheric Composition Change (NDACC) can be combined with near-infrared (NIR) soundings from the Total Carbon Column Observing Network (TCCON) without the need to apply an overall intercalibration factor. However, in spite of efforts to reduce a priori impact, some residual seasonal biases were identified, and the reasons behind remained unclear. In extension to this previous work, which was based on multiannual quasi-coincident MIR and NIR measurements from the stations Garmisch (47.48° N, 11.06° E, 743 m a.s.l.) and Wollongong (34.41° S, 150.88° E, 30 m a.s.l.), we now investigate upgraded retrievals with longer temporal coverage and include three additional stations (Ny-Ålesund, 78.92° N, 11.93° E, 20 m a.s.l.; Karlsruhe, 49.08° N, 8.43° E, 110 m a.s.l.; Izaña, 28.31° N, 16.45° W, 2.370 m a.s.l.). Our intercomparison results (except for Ny-Ålesund) confirm that there is no overall bias between MIR and NIR XCH 4 retrievals, and all MIR and NIR time series reveal a quasi-periodic seasonal bias for all stations, except for Izaña. We find that dynamical variability causes MIR–NIR differences of up to ~ 30 ppb (parts per billion) for Ny-Ålesund, ~ 20 ppb for Wollongong, ~ 18 ppb for Garmisch, and ~ 12 ppb for Karlsruhe. The mechanisms behind this variability are elaborated via two case studies, one dealing with stratospheric subsidence induced by the polar vortex at Ny-Ålesund and the other with a deep stratospheric intrusion event at Garmisch. Smoothing effects caused by the dynamical variability during these events are different for MIR and NIR retrievals depending on the altitude of the perturbation area. MIR retrievals appear to be more realistic in the case of stratospheric subsidence, while NIR retrievals are more accurate in the case of stratosphere–troposphere exchange (STE) in the upper troposphere/lower stratosphere (UTLS) region. About 35% of the FTIR measurement days at Garmisch are impacted by STE, and about 23% of the measurement days at Ny-Ålesund are influenced by polar vortex subsidence. The exclusion of data affected by these dynamical situations resulted in improved agreement of MIR and NIR seasonal cycles for Ny-Ålesund and Garmisch. We found that dynamical variability is a key factor in constraining the accuracy of MIR and NIR seasonal cycles. To mitigate this impact it is necessary to use more realistic a priori profiles that take these dynamical events into account (e.g., via improved models), and/or to improve the FTIR retrievals to achieve a more uniform sensitivity at all altitudes (possibly including profile retrievals for the TCCON data).

Description: Technical Note: Probabilistically constraining proxy age–depth models within a Bayesian hierarchical reconstruction model Climate of the Past Discussions, 10, 4499-4533, 2014 Author(s): J. P. Werner and M. P. Tingley Reconstructions of late-Holocene climate rely heavily upon proxies that are assumed to be accurately dated by layer counting, such as measurement on tree rings, ice cores, and varved lake sediments. Considerable advances may be achievable if time uncertain proxies could be included within these multiproxy reconstructions, and if time uncertainties were recognized and correctly modeled for proxies commonly treated as free of age model errors. Current approaches to accounting for time uncertainty are generally limited to repeating the reconstruction using each of an ensemble of age models, thereby inflating the final estimated uncertainty – in effect, each possible age model is given equal weighting. Uncertainties can be reduced by exploiting the inferred space–time covariance structure of the climate to re-weight the possible age models. Here we demonstrate how Bayesian Hierarchical climate reconstruction models can be augmented to account for time uncertain proxies. Critically, while a priori all age models are given equal probability of being correct, the probabilities associated with the age models are formally updated within the Bayesian framework, thereby reducing uncertainties. Numerical experiments show that updating the age-model probabilities decreases uncertainty in the climate reconstruction, as compared with the current de-facto standard of sampling over all age models, provided there is sufficient information from other data sources in the region of the time-uncertain proxy. This approach can readily be generalized to non-layer counted proxies, such as those derived from marine sediments.

Description: High-resolution records of the beryllium-10 solar activity proxy in ice from Law Dome, East Antarctica: measurement, reproducibility and principal trends Climate of the Past Discussions, 7, 677-713, 2011 Author(s): J. B. Pedro, A. M. Smith, K. J. Simon, T. D. van Ommen, and M. A. J. Curran Three near-monthly resolution 10 Be records are presented from the Dome Summit South (DSS) ice core site, Law Dome, East Antarctica. The chemical preparation and Accelerator Mass Spectrometer (AMS) measurement of these records is described. The reproducibility of 10 Be records at DSS is assessed through intercomparison of the ice core data with data from two previously published and contemporaneous snow pits. We find generally good agreement between the five records, comparable to that observed between other trace chemical records from the site. This result allays concerns raised by a previous Antarctic study (Moraal et al., 2005) about poor reproducibility of ice core 10 Be records. A single composite series is constructed from the three ice cores providing a monthly-resolved record of 10 Be concentrations at DSS over the past decade (1999 to 2009). To our knowledge, this is the first published ice core data spanning the recent exceptional solar minimum of solar cycle 23. 10 Be concentrations are significantly correlated to the cosmic ray flux recorded by the McMurdo neutron monitor ( r xy = 0.64, with 95% CI of 0.53 to 0.71), suggesting that solar modulation of the atmospheric production rate may explain up to ~40% of the variance in 10 Be concentrations at DSS. Sharp concentration peaks occur in most years during the summer-to-autumn, possibly caused by stratospheric incursions. Our results underscore the presence of both production and meteorological signals in ice core 10 Be data.

Description: Tracking climate variability in the western Mediterranean during the Late Holocene: a multiproxy approach Climate of the Past Discussions, 7, 635-675, 2011 Author(s): V. Nieto-Moreno, F. Martínez-Ruiz, S. Giralt, F. Jiménez-Espejo, D. Gallego-Torres, M. Rodrigo-Gámiz, J. García-Orellana, M. Ortega-Huertas, and G. J. de Lange Climate variability in the western Mediterranean is reconstructed for the last 4000 yr using marine sediments recovered in the west Algerian-Balearic basin, near the Alboran basin. Fluctuations in chemical and mineralogical sediment composition as well as grain size distribution are linked to fluvial-eolian oscillations, changes in redox conditions and paleocurrent intensity. Multivariate analyses allowed us to characterize three main groups of geochemical and mineralogical proxies determining the sedimentary record of this region. These three statistical groups were applied to reconstruct paleoclimate conditions at high resolution during the Late Holocene. An increase in fluvial-derived elements (Rb/Al, Ba/Al, REE/Al, Si/Al, Ti/Al, Mg/Al and K/Al ratios), finer grain size, slower flows and oxygen-poor bottom waters – as suggested by sortable silt (10–63 μm), clays ( 〈 2 μm) and redox-sensitive elements (V/Al, Cr/Al, Ni/Al and Zn/Al ratios) – depict the Roman Humid Period (RHP) and the Little Ice Age (LIA), while drier environmental conditions are recognized during the Late Bronze Age-Iron Age (LBA-IA) and the Medieval Warm Period (MWP). Although no Ba excess was registered, other paleoproductivity indicators (total organic carbon content, Br/Al ratio, and organometallic ligands such as U and Cu) display the highest values during the RHP, this period exhibiting by far the most intense productivity of the last 4000 yr. These marine sediments evidence oscillations that support the link of the westernmost Mediterranean climate with the North Atlantic coupled ocean-atmosphere climatic system, pointing to solar irradiance and the North Atlantic Oscillation (NAO) variability as the main driving mechanisms behind natural climate variability over decadal to centennial time-scales for the last 4000 yr.

Description: Assessment of BSRN radiation records for the computation of monthly means Atmospheric Measurement Techniques, 4, 339-354, 2011 Author(s): A. Roesch, M. Wild, A. Ohmura, E. G. Dutton, C. N. Long, and T. Zhang The integrity of the Baseline Surface Radiation Network (BSRN) radiation monthly averages are assessed by investigating the impact on monthly means due to the frequency of data gaps caused by missing or discarded high time resolution data. The monthly statistics, especially means, are considered to be important and useful values for climate research, model performance evaluations and for assessing the quality of satellite (time- and space-averaged) data products. The study investigates the spread in different algorithms that have been applied for the computation of monthly means from 1-min values. The paper reveals that the computation of monthly means from 1-min observations distinctly depends on the method utilized to account for the missing data. The intra-method difference generally increases with an increasing fraction of missing data. We found that a substantial fraction of the radiation fluxes observed at BSRN sites is either missing or flagged as questionable. The percentage of missing data is 4.4%, 13.0%, and 6.5% for global radiation, direct shortwave radiation, and downwelling longwave radiation, respectively. Most flagged data in the shortwave are due to nighttime instrumental noise and can reasonably be set to zero after correcting for thermal offsets in the daytime data. The study demonstrates that the handling of flagged data clearly impacts on monthly mean estimates obtained with different methods. We showed that the spread of monthly shortwave fluxes is generally clearly higher than for downwelling longwave radiation. Overall, BSRN observations provide sufficient accuracy and completeness for reliable estimates of monthly mean values. However, the value of future data could be further increased by reducing the frequency of data gaps and the number of outliers. It is shown that two independent methods for accounting for the diurnal and seasonal variations in the missing data permit consistent monthly means to within less than 1 W m −2 in most cases. The authors suggest using a standardized method for the computation of monthly means which addresses diurnal variations in the missing data in order to avoid a mismatch of future published monthly mean radiation fluxes from BSRN. The application of robust statistics would probably lead to less biased results for data records with frequent gaps and/or flagged data and outliers. The currently applied empirical methods should, therefore, be completed by the development of robust methods.

Description: Impact of maximum borehole depths on inverted temperature histories in borehole paleoclimatology Climate of the Past Discussions, 7, 715-748, 2011 Author(s): H. Beltrami, J. E. Smerdon, G. S. Matharoo, and N. Nickerson A quantitative assessment is presented for the impact of the maximum depth of a temperature-depth profile on the estimate of the climatic transient and the resultant ground surface temperature (GST) reconstruction used in borehole paleoclimatology. The depth of the profile is important because the downwelling climatic signal must be separated from the quasi-steady state thermal regime established by the energy in the Earth's interior. This component of the signal is estimated as a linear increase in temperature with depth from the lower section of a borehole temperature profile, which is assumed to be unperturbed by recent changes in climate at the surface. The validity of this assumption is dependent on both the subsurface thermophysical properties and the character of the downwelling climatic signal. Such uncertainties can significantly impact the determination of the quasi-steady state thermal regime, and consequently the magnitude of the temperature anomaly interpreted as a climatic signal. The quantitative effects and uncertainties that arise from the analysis of temperature-depth profiles of different depths are presented. Results demonstrate that widely different GST histories can be derived from a single temperature profile truncated at different depths. Borehole temperature measurements approaching 500–600 m depths are shown to provide the most robust GST reconstructions spanning 500 to 1000 ybp. It is further shown that the bias introduced by a temperature profile of depths shallower than 500–600 m remains even if the time span of the reconstruction target is shortened.