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: 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: 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: 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: 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: 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: 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: 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: 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: Online atmospheric pressure chemical ionization ion trap mass spectrometry (APCI-IT-MS n ) for measuring organic acids in concentrated bulk aerosol – a laboratory and field study Atmospheric Measurement Techniques, 6, 431-443, 2013 Author(s): A. L. Vogel, M. Äijälä, M. Brüggemann, M. Ehn, H. Junninen, T. Petäjä, D. R. Worsnop, M. Kulmala, J. Williams, and T. Hoffmann The field application of an aerosol concentrator in conjunction with an atmospheric pressure chemical ionization ion trap mass spectrometer (APCI-IT-MS) at the boreal forest station SMEAR II at Hyytiälä, Finland, is demonstrated in this study. APCI is a soft-ionization technique allowing online measurements of organic acids in the gas and particle phase. The detection limit for the acid species in the particle phase was improved by a factor of 7.5 to 11 (e.g. ∼40 ng m 3 for pinonic acid) by using the miniature versatile aerosol concentration enrichment system (mVACES) upstream of the mass spectrometer. The APCI-IT-MS was calibrated in the negative ion mode with two biogenic organic acid standards – pinic acid and pinonic acid. Pinic acid was used as a surrogate for the quantification of the total amount of organic acids in the ambient aerosol based on the total signal intensities in the negative ion mode. The results were compared with the total organic signal of a C-ToF-AMS during the HUMPPA-COPEC 2010 field campaign. The campaign average contribution of organic acids measured by APCI-IT-MS to the total submicron organic aerosol mass was estimated to be about 60%, based on the response of pinic acid. Very good correlation between APCI-IT-MS and C-ToF-AMS (Pearson's R = 0.94) demonstrates soft-ionization mass spectrometry as a complimentary technique to AMS with electron impact ionization. MS 2 studies of specific m/z ratios recorded during the HUMPPA-COPEC 2010 field campaign were compared to MS 2 studies of selected monoterpene oxidation products formed in simulation chamber experiments. The comparison of the resulting fragments shows that oxidation products of the main VOCs emitted at Hyytiälä (α-pinene and Δ 3 -carene) cannot account for all of the measured fragments. Possible explanations for those unaccounted fragments are the presence of unidentified or underestimated biogenic SOA precursors, or that different products are formed by a different oxidant mixture of the ambient air compared to the chamber ozonolysis.

Description: First intercalibration of column-averaged methane from the Total Carbon Column Observing Network and the Network for the Detection of Atmospheric Composition Change Atmospheric Measurement Techniques, 6, 397-418, 2013 Author(s): R. Sussmann, A. Ostler, F. Forster, M. Rettinger, N. M. Deutscher, D. W. T. Griffith, J. W. Hannigan, N. Jones, and P. K. Patra We present the first intercalibration of dry-air column-averaged mole fractions of methane (XCH 4 ) retrieved from solar Fourier transform infrared (FTIR) measurements of the Network for the Detection of Atmospheric Composition Change (NDACC) in the mid-infrared (MIR) versus near-infrared (NIR) soundings from the Total Carbon Column Observing Network (TCCON). The study uses multi-annual quasi-coincident MIR and NIR measurements from the stations Garmisch, Germany (47.48° N, 11.06° E, 743 m a.s.l.), and Wollongong, Australia (34.41° S, 150.88° E, 30 m a.s.l.). Direct comparison of the retrieved MIR and NIR XCH 4 time series for Garmisch shows a quasi-periodic seasonal bias leading to a standard deviation (stdv) of the difference time series (NIR–MIR) of 7.2 ppb. After reducing time-dependent a priori impact by using realistic site- and time-dependent ACTM-simulated profiles as a common prior, the seasonal bias is reduced (stdv = 5.2 ppb). A linear fit to the MIR/NIR scatter plot of monthly means based on same-day coincidences does not show a y -intercept that is statistically different from zero, and the MIR/NIR intercalibration factor is found to be close to ideal within 2-σ uncertainty, i.e. 0.9996(8). The difference time series (NIR–MIR) do not show a significant trend. The same basic findings hold for Wollongong. In particular an overall MIR/NIR intercalibration factor close to the ideal 1 is found within 2-σ uncertainty. At Wollongong the seasonal cycle of methane is less pronounced and corresponding smoothing errors are not as significant, enabling standard MIR and NIR retrievals to be used directly, without correction to a common a priori. Our results suggest that it is possible to set up a harmonized NDACC and TCCON XCH 4 data set which can be exploited for joint trend studies, satellite validation, or the inverse modeling of sources and sinks.

Description: Comparison between MODIS and AIRS/AMSU satellite-derived surface skin temperatures Atmospheric Measurement Techniques, 6, 445-455, 2013 Author(s): Y.-R. Lee, J.-M. Yoo, M.-J. Jeong, Y.-I. Won, T. Hearty, and D.-B. Shin Surface skin temperatures of the Level 3 products of MODIS Collection 5 (C5) and AIRS/AMSU version 5 (V5) have been compared in terms of monthly anomaly trends and climatologies over the globe during the period from September 2002 to August 2011. The MODIS temperatures in the 50° N–50° S region tend to systematically be ~1.7 K colder over land and ~0.5 K warmer over ocean than the AIRS/AMSU temperatures. Over high latitude ocean the MODIS sea surface temperature (SST) values are ~5.5 K warmer than the AIRS/AMSU. The discrepancies between the annual averages of the two sensors are as much as ~12 K in the sea ice regions. Meanwhile, the MODIS ice surface temperature product (MYD29E1D) over the ocean is in better agreement with AIRS/AMSU temperatures, showing a root mean square error of 3.7–3.9 K. The disagreement between the two sensors results mainly from the differences in ice/snow emissivity between MODIS infrared and AMSU microwave, and also in their observational local times. Both MODIS and AIRS/AMSU show cooling rates from −0.05 ± 0.06 to −0.14 ± 0.07 K 9 yr −1 over the globe, but warming rates (0.02 ± 0.12 –0.15 ± 0.19 K 9 yr −1 ) in the high latitude regions.

Description: Position error in profiles retrieved from MIPAS observations with a 1-D algorithm Atmospheric Measurement Techniques, 6, 419-429, 2013 Author(s): M. Carlotti, E. Arnone, E. Castelli, B. M. Dinelli, and E. Papandrea The information load (IL) analysis, first introduced for the two-dimensional approach (Carlotti and Magnani, 2009), is applied to the inversion of MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) observations operated with a 1-dimensional (1-D) retrieval algorithm. The IL distribution of MIPAS spectra is shown to be often asymmetrical with respect to the tangent points of the observations and permits us to define the preferential latitude where the profiles retrieved with a 1-D algorithm should be geo-located. Therefore, defining the geo-location of the retrieved profile by means of the tangent points leads to a "position error". We assess the amplitude of the position error for some of the MIPAS main products and we show that the IL analysis can also be used as a tool for the selection of spectral intervals that, when analyzed, minimize the position error of the retrieved profile. When the temperature ( T ) profiles are used for the retrieval of volume mixing ratio (VMR) of atmospheric constituents, the T -position error (of the order of 1.5 degrees of latitude) induces a VMR error that is directly connected with the horizontal T gradients. Temperature profiles can be externally-provided or determined in a previous step of the retrieval process. In the first case, the IL analysis shows that a meaningful fraction (often exceeding 50%) of the VMR error deriving from the 1-D approximation is to be attributed to the mismatch between the position assigned to the external T profile and the positions where T is required by the analyzed observations. In the second case the retrieved T values suffer by an error of 1.5–2 K due to neglecting the horizontal variability of T ; however the error induced on VMRs is of minor concern because of the generally small mismatch between the IL distribution of the observations analyzed to retrieve T and those analyzed to retrieve the VMR target. An estimate of the contribution of the T -position error to the error budget is provided for MIPAS main products. This study shows that the information load analysis can be successfully exploited in a 1-D context that makes the assumption of horizontal homogeneity of the analyzed portion of atmosphere. The analysis that we propose can be extended to the 1-D inversion of other limb-sounding experiments.

Description: Cirrus crystal fall velocity estimates using the Match method with ground-based lidars: first investigation through a case study Atmospheric Measurement Techniques, 6, 457-470, 2013 Author(s): D. Dionisi, P. Keckhut, C. Hoareau, N. Montoux, and F. Congeduti Cirrus ice particle sedimentation velocity ( v s ) is one of the critical variables for the parameterization of cirrus properties in a global climate model (GCM). In this study a methodology to estimate cirrus properties, such as crystal mean fall speed, through successive lidar measurements is evaluated. This "Match" technique has been applied on cirrus cloud observations and then tested with measurements from two ground-based lidars located in the Mediterranean area. These systems, with similar instrumental characteristics, are installed at the Observatory of Haute Provence (OHP, 43.9° N, 5.7° E) in France and at Rome Tor Vergata (RTV, 41.8° N, 12.6° E) in Italy. At a distance of approximately 600 km, the two lidar stations have provided systematic measurements for several years and are along a typical direction of an air path. A test case of an upper tropospheric cirrus, observed over both sites during the night between 13 and 14 March 2008, has been selected and the feasibility of the Match-cirrus approach investigated through this case. The analysis through lidar principal parameters (vertical location, geometrical thickness and optical depth) reveals a case of a thin sub-visible cirrus (SVC) located around the tropopause. A first range of values for v s (1.4–1.9 cm s −1 , consistent with simple-shaped small crystals) has been retrieved with a simplified approach (adiabatic transport and "frozen" microphysical conditions inside the cirrus). The backward trajectory analysis suggests a type of cirrus formed by large-scale transport processes (adiabatic cooling of moist air masses coming from the subtropical area around Mexico gulf), which is characterized by a long atmospheric lifetime and horizontal extension of several hundred km. The analysis of this case study reveals that many uncertainties reduce the confidence of the retrieved estimates of the crystal fall velocity. However, this paper allows for assessing the technique feasibility by identifying the main critical issues for future similar investigations. This study shows that such approach is feasible; however, the methodology should be improved and some directions have been suggested for future campaigns.

Description: Aerosol optical depth (AOD) retrieval using simultaneous GOES-East and GOES-West reflected radiances over the western United States Atmospheric Measurement Techniques, 6, 471-486, 2013 Author(s): H. Zhang, R. M. Hoff, S. Kondragunta, I. Laszlo, and A. Lyapustin Aerosol optical depth (AOD) in the western United States is observed independently by both the (Geostationary Operational Environmental Satellites) GOES-East and GOES-West imagers. The GASP (GOES Aerosol/Smoke Product) aerosol optical depth retrieval algorithm treats each satellite as a unique sensor and thus obtains two separate aerosol optical depth values at the same time for the same location. The TOA (the top of the atmosphere) radiances and the associated derived optical depths can be quite different due to the different viewing geometries with large difference in solar-scattering angles. In order to fully exploit the simultaneous observations and generate consistent AOD retrievals from the two satellites, the authors develop a new "hybrid" aerosol optical depth retrieval algorithm that uses data from both satellites. The algorithm uses both GOES-East and GOES-West visible channel TOA reflectance and daily average AOD from GOES Multi-Angle Implementation of Atmospheric Correction (GOES-MAIAC) on low AOD days (AOD less than 0.3), when diurnal variation of AOD is low, to retrieve surface BRDF (Bidirectional Reflectance Distribution Function). The known BRDF shape is applied on subsequent days to retrieve BRDF and AOD. The algorithm is validated at three AERONET sites over the western US. The AOD retrieval accuracy from the "hybrid" technique using the two satellites is similar to that from one satellite over UCSB (University of California Santa Barbara) and Railroad Valley, Nevada. Improvement of the accuracy is observed at Boulder, Colorado. The correlation coefficients between the GOES AOD and AERONET AOD are in the range of 0.67 to 0.81. More than 74% of AOD retrievals are within the error of ±(0.05 + 0.15 τ) compared to AERONET AOD. The hybrid algorithm has more data coverage compared to the single satellite retrievals over surfaces with high surface reflectance. For single observation areas the number of valid AOD data increases from the use of two-single satellite algorithms by 5–80% for the three sites. With the application of the new algorithm, consistent AOD retrievals and better retrieval coverages can be obtained using the data from the two GOES satellite imagers.

Description: Retrieval and satellite intercomparison of O 3 measurements from ground-based FTIR Spectrometer at Equatorial Station: Addis Ababa, Ethiopia Atmospheric Measurement Techniques, 6, 495-509, 2013 Author(s): S. Takele Kenea, G. Mengistu Tsidu, T. Blumenstock, F. Hase, T. von Clarmann, and G. P. Stiller Since May 2009, high-resolution Fourier Transform Infrared (FTIR) solar absorption spectra have been recorded at Addis Ababa (9.01° N latitude, 38.76° E longitude, 2443 m altitude above sea level), Ethiopia. The vertical profiles and total column amounts of ozone (O 3 ) are deduced from the spectra by using the retrieval code PROFFIT (V9.5) and regularly determined instrumental line shape (ILS). A detailed error analysis of the O 3 retrieval is performed. Averaging kernels of the target gas shows that the major contribution to the retrieved information comes from the measurement. The degrees of freedom for signals is found to be 2.1 on average for the retrieval of O 3 from the observed FTIR spectra. The ozone Volume Mixing Ratio (VMR) profiles and column amounts retrieved from FTIR spectra are compared with the coincident satellite observations of Microwave Limb Sounding (MLS), Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), Tropospheric Emission Spectrometer (TES), Ozone Monitoring Instrument (OMI), Atmospheric Infrared Sounding (AIRS) and Global Ozone Monitoring Experiment (GOME-2) instruments. The mean relative differences in ozone profiles of FTIR from MLS and MIPAS are generally lower than 15% within the altitude range of 27 to 36 km, whereas difference from TES is lower than 1%. Comparisons of measurements of column amounts from the satellite and the ground-based FTIR show very good agreement as exhibited by relative differences within +0.2% to +2.8% for FTIR versus MLS and GOME-2; and −0.9 to −9.0% for FTIR versus OMI, TES and AIRS. The corresponding standard deviations are within 2.0 to 2.8% for FTIR versus MLS and GOME-2 comparisons whereas that of FTIR versus OMI, TES and AIRS are within 3.5 to 7.3%. Thus, the retrieved O 3 VMR and column amounts from a tropical site, Addis Ababa, is found to exhibit very good agreement with all coincident satellite observations over an approximate 3-yr period.

Description: Influence of spatial heterogeneity of local surface albedo on the area-averaged surface albedo retrieved from airborne irradiance measurements Atmospheric Measurement Techniques, 6, 527-537, 2013 Author(s): E. Jäkel, M. Wendisch, and B. Mayer Spectral airborne upward and downward irradiance measurements are used to derive the area-averaged surface albedo. Real surfaces are not homogeneous in their reflectivity. Therefore, this work studies the effects of the heterogeneity of surface reflectivity on the area-averaged surface albedo to quantify how well aircraft measurements can resolve the small-scale variability of the local surface albedo. For that purpose spatially heterogeneous surface albedo maps were input into a 3-dimensional (3-D) Monte Carlo radiative transfer model to simulate 3-D irradiance fields. The calculated up- and downward irradiances in altitudes between 0.1 and 5 km are used to derive the area-averaged surface albedo using an iterative retrieval method that removes the effects due to atmospheric scattering and absorption within the layer beneath the considered level. For the case of adjacent land and sea surfaces, parametrizations are presented which quantify the horizontal distance from the coastline that is required to reduce surface heterogeneity effects on the area-averaged surface albedo to a given limit. The parametrization which is a function of altitude, aerosol optical depth, single scattering albedo, and the ratio of local land and sea albedo was applied for airborne spectral measurements. In addition, the deviation between area-averaged and local surface albedo is determined for more complex surface albedo maps. For moderate aerosol conditions (optical depth less than 0.4) and a wavelength range between 400 and 1000 nm, the altitude and the heterogeneity of the surface albedo are the dominant factors determining the mean deviation between local and area-averaged surface albedo. A parametrization of the mean deviation is applied to an albedo map that was derived from a Landsat image of an area in East Anglia (UK). Parametrization and direct comparison of local and area-averaged surface albedo show similar mean deviations (20% vs. 25%) over land.

Description: Thermodynamic phase retrieval of convective clouds: impact of sensor viewing geometry and vertical distribution of cloud properties Atmospheric Measurement Techniques, 6, 539-547, 2013 Author(s): E. Jäkel, J. Walter, and M. Wendisch The sensitivity of passive remote sensing measurements to retrieve microphysical parameters of convective clouds, in particular their thermodynamic phase, is investigated by three-dimensional (3-D) radiative transfer simulations. The effects of different viewing geometries and vertical distributions of the cloud microphysical properties are investigated. Measurement examples of spectral solar radiance reflected by cloud sides (passive) in the near-infrared (NIR) spectral range are performed together with collocated lidar observations (active). The retrieval method to distinguish the cloud thermodynamic phase (liquid water or ice) exploits different slopes of cloud side reflectivity spectra of water and ice clouds in the NIR. The concurrent depolarization backscattering lidar provides geometry information about the cloud distance and height as well as the depolarization.

Description: Improvements to the retrieval of tropospheric NO 2 from satellite – stratospheric correction using SCIAMACHY limb/nadir matching and comparison to Oslo CTM2 simulations Atmospheric Measurement Techniques, 6, 565-584, 2013 Author(s): A. Hilboll, A. Richter, A. Rozanov, Ø. Hodnebrog, A. Heckel, S. Solberg, F. Stordal, and J. P. Burrows Satellite measurements of atmospheric trace gases have proved to be an invaluable tool for monitoring the Earth system. When these measurements are to be used for assessing tropospheric emissions and pollution, as for example in the case of nadir measurements of nitrogen dioxide (NO 2 ), it is necessary to separate the stratospheric from the tropospheric signal. The SCIAMACHY instrument offers the unique opportunity to combine its measurements in limb- and nadir-viewing geometries into a tropospheric data product, using the limb measurements of the stratospheric NO 2 abundances to correct the nadir measurements' total columns. In this manuscript, we present a novel approach to limb/nadir matching, calculating one stratospheric NO 2 value from limb measurements for every single nadir measurement, abandoning global coverage for the sake of spatial accuracy. For comparison, modelled stratospheric NO 2 columns from the Oslo CTM2 are also evaluated for stratospheric correction. Our study shows that stratospheric NO 2 columns from SCIAMACHY limb measurements very well reflect stratospheric conditions. The zonal variability of the stratospheric NO 2 field is captured by our matching algorithm, and the quality of the resulting tropospheric NO 2 columns improves considerably. Both stratospheric datasets need to be adjusted to the level of the nadir measurements, because a time- and latitude-dependent bias to the measured nadir columns can be observed over clean regions. After this offset is removed, the two datasets agree remarkably well, and both stratospheric correction methods provide a significant improvement to the retrieval of tropospheric NO 2 columns from the SCIAMACHY instrument.

Description: Quantification of uncertainties of water vapour column retrievals using future instruments Atmospheric Measurement Techniques, 6, 359-370, 2013 Author(s): H. Diedrich, R. Preusker, R. Lindstrot, and J. Fischer This study presents a quantification of uncertainties of total column water vapour retrievals based on simulated near-infrared measurements of upcoming instruments. The concepts of three scheduled spectrometers were taken into account: OLCI (Ocean and Land Color Instrument) on Sentinel-3, METimage on an EPS-SG (EUMETSAT Polar System – Second Generation) satellite and FCI (Flexible Combined Imager) on MTG (Meteosat Third Generation). Optimal estimation theory was used to estimate the error of a hypothetical total water vapour column retrieval for 27 different atmospheric cases. The errors range from 100% in very dry cases to 2% in humid cases with a very high surface albedo. Generally, the absolute uncertainties increase with higher water vapour column content due to H 2 O-saturation and decrease with a brighter surface albedo. Uncertainties increase with higher aerosol optical thickness, apart from very dark cases. Overall, the METimage channel setting enables the most accurate retrievals. The retrieval using the MTG-FCI build-up has the highest uncertainties apart from very bright cases. On the one hand, a retrieval using two absorption channels increases the accuracy, in some cases by one order of magnitude, in comparison to a retrieval using just one absorption channel. On the other hand, a retrieval using three absorption channels has no significant advantage over a two-absorption channel retrieval. Furthermore, the optimal position of the absorption channels was determined using the concept of the "information content". For a single channel retrieval, a channel at 900 or 915 nm has the highest mean information content over all cases. The second absorption channel is ideally weakly correlated with the first one, and therefore positioned at 935 nm, in a region with stronger water vapour absorption.

Description: Characterisation of GOME-2 formaldehyde retrieval sensitivity Atmospheric Measurement Techniques, 6, 371-386, 2013 Author(s): W. Hewson, H. Bösch, M. P. Barkley, and I. De Smedt Formaldehyde (CH 2 O) is an important tracer of tropospheric photochemistry, whose slant column abundance can be retrieved from satellite measurements of solar backscattered UV radiation, using differential absorption retrieval techniques. In this work a spectral fitting sensitivity analysis is conducted on CH 2 O slant columns retrieved from the Global Ozone Monitoring Experiment 2 (GOME-2) instrument. Despite quite different spectral fitting approaches, the retrieved CH 2 O slant columns have geographic distributions that generally match expected CH 2 O sources, though the slant column magnitudes and corresponding uncertainties are particularly sensitive to the retrieval set-up. The choice of spectral fitting window, polynomial order, I 0 correction, and inclusion of minor absorbers tend to result in the largest modulations of retrieved slant column magnitude and fit quality. However, application of a reference sector correction using observations over the remote Pacific Ocean is shown to largely homogenise the resulting CH 2 O vertical columns obtained with different retrieval settings, thereby largely reducing any systematic error sources from spectral fitting.

Description: Retrieval interval mapping: a tool to visualize the impact of the spectral retrieval range on differential optical absorption spectroscopy evaluations Atmospheric Measurement Techniques, 6, 275-299, 2013 Author(s): L. Vogel, H. Sihler, J. Lampel, T. Wagner, and U. Platt Remote sensing via differential optical absorption spectroscopy (DOAS) has become a standard technique to identify and quantify trace gases in the atmosphere. Due to the wide range of measurement conditions, atmospheric compositions and instruments used, a specific challenge of a DOAS retrieval is to optimize the retrieval parameters for each specific case and particular trace gas of interest. Of these parameters, the retrieval wavelength range is one of the most important ones. Although for many trace gases the overall dependence of common DOAS retrieval on the evaluation wavelength interval is known, a systematic approach for finding the optimal retrieval wavelength range and quantitative assessment is missing. Here we present a novel tool to visualize the effect of different evaluation wavelength ranges. It is based on mapping retrieved column densities in the retrieval wavelength space and thus visualizing the consequences of different choices of spectral retrieval ranges caused by slightly erroneous absorption cross sections, cross correlations and instrumental features. Based on the information gathered, an optimal retrieval wavelength range may be determined systematically. The technique is demonstrated using examples of a theoretical study of BrO retrievals for stratospheric BrO and BrO measurements in volcanic plumes. However, due to the general nature of the tool, it is applicable to any type of DOAS retrieval (active or passive).

Description: Water vapor isotopologue retrievals from high-resolution GOSAT shortwave infrared spectra Atmospheric Measurement Techniques, 6, 263-274, 2013 Author(s): C. Frankenberg, D. Wunch, G. Toon, C. Risi, R. Scheepmaker, J.-E. Lee, P. Wennberg, and J. Worden Remote sensing of the isotopic composition of water vapor can provide valuable information on the hydrological cycle. Here, we demonstrate the feasibility of retrievals of the relative abundance of HDO (the HDO/H 2 O ratio) from the Japanese GOSAT satellite. For this purpose, we use high spectral resolution nadir radiances around 6400 cm −1 (1.56 μm) to retrieve vertical column amounts of H 2 O and HDO. Retrievals of H 2 O correlate well with ECMWF (European Centre for Medium-Range Weather Forecasts) integrated profiles ( r 2 = 0.96). Typical precision errors in the retrieved column-averaged deuterium depletion (δD) are 20–40‰. We compare δD against a TCCON (Total Carbon Column Observing Network) ground-based station in Lamont, Oklahoma. Using retrievals in very dry areas over Antarctica, we detect a small systematic offset in retrieved H 2 O and HDO column amounts and take this into account for a bias correction of δD. Monthly averages of δD in the June 2009 to September 2011 time frame are well correlated with TCCON ( r 2 = 0.79) and exhibit a slope of 0.98 (1.23 if not bias corrected). We also compare seasonal averages on the global scale with results from the SCIAMACHY instrument in the 2003–2005 time frame. Despite the lack of temporal overlap, seasonal averages in general agree well, with spatial correlations ( r 2 ) ranging from 0.62 in September through November to 0.83 in June through August. However, we observe higher variability in GOSAT δD, indicated by fitted slopes between 1.2 and 1.46. The discrepancies are likely related to differences in vertical sensitivities but warrant further validation of both GOSAT and SCIAMACHY and an extension of the validation dataset.

Description: An improved cirrus detection algorithm MeCiDA2 for SEVIRI and its evaluation with MODIS Atmospheric Measurement Techniques, 6, 309-322, 2013 Author(s): F. Ewald, L. Bugliaro, H. Mannstein, and B. Mayer In this study, a substantially improved version of the Meteosat cirrus detection algorithm (MeCiDA2) will be presented, which now allows application to the full earth disc visible by the Meteosat satellite. As cirrus clouds have an influence on the radiation budget of the earth, their optical properties and their global coverage has to be monitored at the global scale using instruments aboard geostationary satellites. Since MeCiDA was optimised for the area of Europe only, various changes were necessary to handle the variable conditions found over the full Meteosat disc. Required changes include the consideration of the viewing angle dependency and of the sensitivity of the 9.7 μm channel to the ozone column. To this end, a correction is implemented that minimises the influence of the variability of the stratospheric ozone. The evaluation of the proposed improvements is carried out by using MeCiDA applied to MODIS (moderate resolution imaging spectrometer) data to address viewing angle-dependent cirrus detection, and by additionally comparing it to the cloud optical properties MOD06 cirrus product. The new MeCiDA version detects less cirrus than the original one for latitudes larger than 40°, but almost the same amount elsewhere. MeCiDA's version for MODIS is more sensitive than that for SEVIRI (spinning enhanced visible and infrared imager) with cirrus occurrences higher by 10%, and the new MeCiDA provides almost the same cirrus coverage (±0.1) as given by the cloud phase optical properties from MODIS for latitudes smaller than 50°. Finally, the influence of sub-pixel clouds on the SEVIRI cirrus detection has been examined: more than 60% of the undetected SEVIRI cirrus pixels have a cirrus coverage smaller than 0.5.

Description: A centrifugal ice microtome for measurements of atmospheric CO 2 on air trapped in polar ice cores Atmospheric Measurement Techniques, 6, 251-262, 2013 Author(s): B. Bereiter, T. F. Stocker, and H. Fischer For atmospheric CO 2 reconstructions using ice cores, the technique to release the trapped air from the ice samples is essential for the precision and accuracy of the measurements. We present here a new dry extraction technique in combination with a new gas analytical system that together show significant improvements with respect to current systems. Ice samples (3–15 g) are pulverised using a novel centrifugal ice microtome (CIM) by shaving the ice in a cooled vacuum chamber (−27 °C) in which no friction occurs due to the use of magnetic bearings. Both, the shaving principle of the CIM and the use of magnetic bearings have not been applied so far in this field. Shaving the ice samples produces finer ice powder and releases a minimum of 90% of the trapped air compared to 50%–70% when needle crushing is employed. In addition, the friction-free motion with an optimized design to reduce contaminations of the inner surfaces of the device result in a reduced system offset of about 2.0 ppmv compared to 4.9 ppmv. The gas analytical part shows a higher precision than the corresponding part of our previous system by a factor of two, and all processes except the loading and cleaning of the CIM now run automatically. Compared to our previous system, the complete system shows a 3 times better measurement reproducibility of about 1.1 ppmv (1 σ) which is similar to the best reproducibility of other systems applied in this field. With this high reproducibility, no replicate measurements are required anymore for most future measurement campaigns resulting in a possible output of 12–20 measurements per day compared to a maximum of 6 with other systems.

Description: Evaluation of a cavity ring-down spectrometer for in situ observations of 13 CO 2 Atmospheric Measurement Techniques, 6, 301-308, 2013 Author(s): F. R. Vogel, L. Huang, D. Ernst, L. Giroux, S. Racki, and D. E. J. Worthy With the emergence of wide-spread application of new optical techniques to monitor δ 13 C in atmospheric CO 2 there is a growing need to ensure well-calibrated measurements. We characterized one commonly available instrument, a cavity ring-down spectrometer (CRDS) system used for continuous in situ monitoring of atmospheric 13 CO 2 . We found no dependency of δ 13 C on the CO 2 concentration in the range of 303–437 ppm. We designed a calibration scheme according to the diagnosed instrumental drifts and established a quality assurance protocol. We find that the repeatability (1-σ) of measurements is 0.25‰ for 10 min and 0.15‰ for 20 min integrated averages, respectively. Due to a spectral overlap, our instrument displays a cross-sensitivity to CH 4 of 0.42 ± 0.024‰ ppm −1 . Our ongoing target measurements yield standard deviations of δ 13 C from 0.22‰ to 0.28‰ for 10 min averages. We furthermore estimate the reproducibility of our system for ambient air samples from weekly measurements of a long-term target gas to be 0.18‰. We find only a minuscule offset of 0.002 ± 0.025‰ between the CRDS and Environment Canada's isotope ratio mass spectrometer (IRMS) results for four target gases used over the course of one year.

Description: Continuous stand-alone controllable aerosol/cloud droplet dryer for atmospheric sampling Atmospheric Measurement Techniques, 6, 349-357, 2013 Author(s): S. Sjogren, G. P. Frank, M. I. A. Berghof, and B. G. Martinsson We describe a general-purpose dryer designed for continuous sampling of atmospheric aerosol, where a specified relative humidity (RH) of the sample flow (lower than the atmospheric humidity) is required. It is often prescribed to measure the properties of dried aerosol, for instance for monitoring networks. The specific purpose of our dryer is to dry cloud droplets (maximum diameter approximately 25 μm, highly charged, up to 5 × 10 2 charges). One criterion is to minimise losses from the droplet size distribution entering the dryer as well as on the residual dry particle size distribution exiting the dryer. This is achieved by using a straight vertical downwards path from the aerosol inlet mounted above the dryer, and removing humidity to a dry, closed loop airflow on the other side of a semi-permeable GORE-TEX membrane (total area 0.134 m 2 ). The water vapour transfer coefficient, k , was measured to be 4.6 × 10 -7 kg m −2 s −1 % RH −1 in the laboratory (temperature 294 K) and is used for design purposes. A net water vapour transfer rate of up to 1.2 × 10 -6 kg s −1 was achieved in the field. This corresponds to drying a 5.7 L min −1 (0.35 m 3 h −1 ) aerosol sample flow from 100% RH to 27% RH at 293 K (with a drying air total flow of 8.7 L min −1 ). The system was used outdoors from 9 May until 20 October 2010, on the mountain Brocken (51.80° N, 10.67° E, 1142 m a.s.l.) in the Harz region in central Germany. Sample air relative humidity of less than 30% was obtained 72% of the time period. The total availability of the measurement system was 〉94% during these five months.

Description: The effect of hygroscopicity on eddy covariance estimates of sea-spray aerosol fluxes: a comparison of high-rate and bulk correction methods Atmospheric Measurement Techniques, 6, 323-335, 2013 Author(s): D. A. J. Sproson, I. M. Brooks, and S. J. Norris The eddy covariance technique is the most direct of the methods that have been used to measure the flux of sea-spray aerosol between the ocean and atmosphere, but has been applied in only a handful of studies. However, unless the aerosol is dried before the eddy covariance measurements are made, the hygroscopic nature of sea-spray may combine with a relative humidity flux to result in a bias in the calculated aerosol flux. "Bulk" methods have been presented to account for this bias, however, they rely on assumptions of the shape of the aerosol spectra which may not be valid for near-surface measurements of sea-spray. Here we describe a method of correcting aerosol spectra for relative humidity induced size variations at the high frequency (10 Hz) measurement timescale, where counting statistics are poor and the spectral shape cannot be well represented by a simple power law. Such a correction allows the effects of hygroscopicity and relative humidity flux on the aerosol flux to be explicitly evaluated and compared to the bulk corrections, both in their original form and once reformulated to better represent the measured mean aerosol spectra. In general, the bulk corrections – particularly when reformulated for the measured mean aerosol spectra – perform relatively well, producing flux corrections of the right sign and approximate magnitude. However, there are times when the bulk methods either significantly over- or underestimate the required flux correction. We conclude that, where possible, relative humidity corrections should be made at the measurement frequency.

Description: Cluster analysis of WIBS single-particle bioaerosol data Atmospheric Measurement Techniques, 6, 337-347, 2013 Author(s): N. H. Robinson, J. D. Allan, J. A. Huffman, P. H. Kaye, V. E. Foot, and M. Gallagher Hierarchical agglomerative cluster analysis was performed on single-particle multi-spatial data sets comprising optical diameter, asymmetry and three different fluorescence measurements, gathered using two dual Wideband Integrated Bioaerosol Sensors (WIBSs). The technique is demonstrated on measurements of various fluorescent and non-fluorescent polystyrene latex spheres (PSL) before being applied to two separate contemporaneous ambient WIBS data sets recorded in a forest site in Colorado, USA, as part of the BEACHON-RoMBAS project. Cluster analysis results between both data sets are consistent. Clusters are tentatively interpreted by comparison of concentration time series and cluster average measurement values to the published literature (of which there is a paucity) to represent the following: non-fluorescent accumulation mode aerosol; bacterial agglomerates; and fungal spores. To our knowledge, this is the first time cluster analysis has been applied to long-term online primary biological aerosol particle (PBAP) measurements. The novel application of this clustering technique provides a means for routinely reducing WIBS data to discrete concentration time series which are more easily interpretable, without the need for any a priori assumptions concerning the expected aerosol types. It can reduce the level of subjectivity compared to the more standard analysis approaches, which are typically performed by simple inspection of various ensemble data products. It also has the advantage of potentially resolving less populous or subtly different particle types. This technique is likely to become more robust in the future as fluorescence-based aerosol instrumentation measurement precision, dynamic range and the number of available metrics are improved.

Description: An airborne amplitude-modulated 1.57 μm differential laser absorption spectrometer: simultaneous measurement of partial column-averaged dry air mixing ratio of CO 2 and target range Atmospheric Measurement Techniques, 6, 387-396, 2013 Author(s): D. Sakaizawa, S. Kawakami, M. Nakajima, T. Tanaka, I. Morino, and O. Uchino Simultaneous measurements of the partial column-averaged dry air mixing ratio of CO 2 (XCO 2 ) and target range were demonstrated using airborne amplitude-modulated 1.57 μm differential laser absorption spectrometer (LAS). The LAS system is useful for discriminating between ground and cloud return signals and has a demonstrated ability to suppress the impact of integrated aerosol signals on atmospheric CO 2 measurements. A high correlation coefficient ( R ) of 0.987 between XCO 2 observed by LAS and XCO 2 calculated from in situ measurements was obtained. The averaged difference in XCO 2 obtained from LAS and validation data was within 1.5 ppm for all spiral measurements. An interesting vertical profile was observed for both XCO 2LAS and XCO 2val , in which lower altitude CO 2 decreases compared to higher altitude CO 2 attributed to the photosynthesis over grassland in the summer. In the case of an urban area where there are boundary-layer enhanced CO 2 and aerosol in the winter, the difference of XCO 2LAS to XCO 2val is a negative bias of 1.5 ppm, and XCO 2LAS is in agreement with XCO 2val within the measurement precision of 2.4 ppm (1 SD).

Description: Note on the application of planar-fit rotation for non-omnidirectional sonic anemometers Atmospheric Measurement Techniques, 6, 221-229, 2013 Author(s): M. Li, W. Babel, K. Tanaka, and T. Foken For non-omnidirectional sonic anemometers like the Kaijo-Denki DAT 600 TR61A probe, it is shown that separate planar-fit rotations must be used for the undisturbed (open part of the sonic anemometer) and the disturbed sector. This increases the friction velocity while no effect on the scalar fluxes was found. In the disturbed sector, irregular values of − u′ w′ 〈 0 were detected for low wind velocities. Up to a certain extent these results can be transferred to the CSAT3 sonic anemometer (Campbell Scientific Ltd). This study was done for data sets from the Naqu-BJ site on the Tibetan Plateau.

Description: Evaluation of ozone profile and tropospheric ozone retrievals from GEMS and OMI spectra Atmospheric Measurement Techniques, 6, 239-249, 2013 Author(s): J. Bak, J. H. Kim, X. Liu, K. Chance, and J. Kim South Korea is planning to launch the GEMS (Geostationary Environment Monitoring Spectrometer) instrument into the GeoKOMPSAT (Geostationary Korea Multi-Purpose SATellite) platform in 2018 to monitor tropospheric air pollutants on an hourly basis over East Asia. GEMS will measure backscattered UV radiances covering the 300–500 nm wavelength range with a spectral resolution of 0.6 nm. The main objective of this study is to evaluate ozone profiles and stratospheric column ozone amounts retrieved from simulated GEMS measurements. Ozone Monitoring Instrument (OMI) Level 1B radiances, which have the spectral range 270–500 nm at spectral resolution of 0.42–0.63 nm, are used to simulate the GEMS radiances. An optimal estimation-based ozone profile algorithm is used to retrieve ozone profiles from simulated GEMS radiances. Firstly, we compare the retrieval characteristics (including averaging kernels, degrees of freedom for signal, and retrieval error) derived from the 270–330 nm (OMI) and 300–330 nm (GEMS) wavelength ranges. This comparison shows that the effect of not using measurements below 300 nm on retrieval characteristics in the troposphere is insignificant. However, the stratospheric ozone information in terms of DFS decreases greatly from OMI to GEMS, by a factor of ∼2. The number of the independent pieces of information available from GEMS measurements is estimated to 3 on average in the stratosphere, with associated retrieval errors of ~1% in stratospheric column ozone. The difference between OMI and GEMS retrieval characteristics is apparent for retrieving ozone layers above ~20 km, with a reduction in the sensitivity and an increase in the retrieval errors for GEMS. We further investigate whether GEMS can resolve the stratospheric ozone variation observed from high vertical resolution Earth Observing System (EOS) Microwave Limb Sounder (MLS). The differences in stratospheric ozone profiles between GEMS and MLS are comparable to those between OMI and MLS below ~3 hPa (~40 km), except with slightly larger biases and larger standard deviations by up to 5%. At pressure altitudes above ~3 hPa, GEMS retrievals show strong influence of a priori and large differences with MLS, which, however, can be sufficiently improved by using better a priori information. The GEMS-MLS differences show negative biases of less than 4% for stratospheric column ozone, with standard deviations of 1–3%, while OMI retrievals show similar agreements with MLS except for 1% smaller biases at middle and high latitudes. Based on the comparisons, we conclude that GEMS will measure tropospheric ozone and stratospheric ozone columns with accuracy comparable to that of OMI and ozone profiles with slightly worse performance than that of OMI below ~3 hPa.

Description: The detection of nocturnal N 2 O 5 as HNO 3 by alkali- and aqueous-denuder techniques Atmospheric Measurement Techniques, 6, 231-237, 2013 Author(s): G. J. Phillips, U. Makkonen, G. Schuster, N. Sobanski, H. Hakola, and J. N. Crowley The almost total anthropogenic control of the nitrogen cycle has led to wide ranging trans-national and national efforts to quantify the effects of reactive nitrogen on the environment. A number of monitoring techniques have been developed for the measurement of nitric acid and subsequent estimation of nitrogen deposition within large networks and for process studies on shorter measurement campaigns. We discuss the likelihood that many of these techniques are sensitive to another important gas-phase component of oxidized nitrogen: dinitrogen pentoxide (N 2 O 5 ). We present measurements using a MARGA wet annular denuder device alongside measurements of N 2 O 5 with a discussion of evidence from the laboratory and the field which suggests that alkali- and aqueous-denuder measurements are sensitive to the sum of HNO 3 + 2N 2 O 5 . Nocturnal data from these denuder devices should be treated with care before using HNO 3 concentrations derived from these data. This is a systematic error which is highly dependent on ambient conditions and is likely to cause systematic misinterpretation of datasets in periods where N 2 O 5 is significant proportion of NO y . It is also likely that deposition estimates of HNO 3 via data obtained with these methods is compromised to greater and lesser extents depending on the season and environment of the sampling location.

Description: Quality assessment of Automatic Dependent Surveillance Contract (ADS-C) wind and temperature observation from commercial aircraft Atmospheric Measurement Techniques, 6, 199-206, 2013 Author(s): S. de Haan, L. J. Bailey, and J. E. Können Aircraft observations of wind and temperature are very important for upper air meteorology. In this article, the quality of the meteorological information of an Automatic Dependent Surveillance-Contract (ADS-C) message is assessed. The ADS-C messages broadcast by the aircraft are received at air traffic control centres for surveillance and airline control centres for general aircraft and dispatch management. A comparison is performed against a global numerical prediction (NWP) model and wind and temperature observations derived from Enhanced Surveillance (EHS) air-traffic control radar which interrogates all aircraft in selective mode (Mode-S EHS). Almost 16 000 ADS-C reports with meteorological information were compiled from the Royal Dutch Airlines (KLM) database. The length of the data set is 76 consecutive days and started on 1 January 2011. The wind and temperature observations are of good quality when compared to the global NWP forecast fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). Comparison of ADS-C wind and temperature observations against Mode-S EHS derived observations in the vicinity of Amsterdam Airport Schiphol shows that the wind observations are of similar quality and the temperature observations of ADS-C are of better quality than those from Mode-S EHS. However, the current ADS-C data set has a lower vertical resolution than Mode-S EHS. High vertical resolution can be achieved by requesting more ADS-C when aircraft are ascending or descending, but could result in increased data communication costs.

Description: Organic particle types by single-particle measurements using a time-of-flight aerosol mass spectrometer coupled with a light scattering module Atmospheric Measurement Techniques, 6, 187-197, 2013 Author(s): S. Liu, L. M. Russell, D. T. Sueper, and T. B. Onasch Chemical and physical properties of individual ambient aerosol particles can vary greatly, so measuring the chemical composition at the single-particle level is essential for understanding atmospheric sources and transformations. Here we describe 46 days of single-particle measurements of atmospheric particles using a time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS). The light scattering module optically detects particles larger than 180 nm vacuum aerodynamic diameter (130 nm geometric diameter) before they arrive at the chemical mass spectrometer and then triggers the saving of single-particle mass spectra. 271 641 particles were detected and sampled during 237 h of sampling in single-particle mode. By comparing timing of the predicted chemical ion signals from the light scattering measurement with the measured chemical ion signals by the mass spectrometer for each particle, particle types were classified and their number fractions determined as follows: prompt vaporization (46%), delayed vaporization (6%), and null (48%), where null was operationally defined as less than 6 ions per particle. Prompt and delayed vaporization particles with sufficient chemical information (i.e., more than 40 ions per particle) were clustered based on similarity of organic mass spectra (using k -means algorithm) to result in three major clusters: highly oxidized particles (dominated by m/z 44), relatively less oxidized particles (dominated by m/z 43), and particles associated with fresh urban emissions. Each of the three organic clusters had limited chemical properties of other clusters, suggesting that all of the sampled organic particle types were internally mixed to some degree; however, the internal mixing was never uniform and distinct particle types existed throughout the study. Furthermore, the single-particle mass spectra and time series of these clusters agreed well with mass-based components identified (using factor analysis) from simultaneous ensemble-averaged measurements, supporting the connection between ensemble-based factors and atmospheric particle sources and processes. Measurements in this study illustrate that LS-ToF-AMS provides unique information about organic particle types by number as well as mass.

Description: Corrigendum to "MAX-DOAS formaldehyde slant column measurements during CINDI: intercomparison and analysis improvement" published in Atmos. Meas. Tech., 6, 167–185, 2013 Atmospheric Measurement Techniques, 6, 219-219, 2013 Author(s): G. Pinardi, M. Van Roozendael, N. Abuhassan, C. Adams, A. Cede, K. Clémer, C. Fayt, U. Frieß, M. Gil, J. Herman, C. Hermans, F. Hendrick, H. Irie, A. Merlaud, M. Navarro Comas, E. Peters, A. J. M. Piters, O. Puentedura, A. Richter, A. Schönhardt, R. Shaiganfar, E. Spinei, K. Strong, H. Takashima, M. Vrekoussis, T. Wagner, F. Wittrock, and S. Yilmaz No abstract available.

Description: Improved mixing height monitoring through a combination of lidar and radon measurements Atmospheric Measurement Techniques, 6, 207-218, 2013 Author(s): A. D. Griffiths, S. D. Parkes, S. D. Chambers, M. F. McCabe, and A. G. Williams Surface-based radon ( 222 Rn) measurements can be combined with lidar backscatter to obtain a higher quality time series of mixing height within the planetary boundary layer (PBL) than is possible from lidar alone, and a more quantitative measure of mixing height than is possible from only radon. The reason why lidar measurements are improved is that there are times when lidar signals are ambiguous, and reliably attributing the mixing height to the correct aerosol layer presents a challenge. By combining lidar with a mixing length scale derived from a time series of radon concentration, automated and robust attribution is possible during the morning transition. Radon measurements provide mixing information during the night, but concentrations also depend on the strength of surface emissions. After processing radon in combination with lidar, we obtain nightly measurements of radon emissions and are able to normalise the mixing length scale for changing emissions. After calibration with lidar, the radon-derived equivalent mixing height agrees with other measures of mixing on daily and hourly timescales and is a potential method for studying intermittent mixing in nocturnal boundary layers.

Description: Comparison of SMILES ClO profiles with satellite, balloon-borne and ground-based measurements Atmospheric Measurement Techniques, 6, 3325-3347, 2013 Author(s): H. Sagawa, T. O. Sato, P. Baron, E. Dupuy, N. Livesey, J. Urban, T. von Clarmann, A. de Lange, G. Wetzel, B. J. Connor, A. Kagawa, D. Murtagh, and Y. Kasai We evaluate the quality of ClO profiles derived from the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station (ISS). Version 2.1.5 of the level-2 product generated by the National Institute of Information and Communications Technology (NICT) is the subject of this study. Based on sensitivity studies, the systematic error was estimated as 5–10 pptv at the pressure range of 80–20 hPa, 35 pptv at the ClO peak altitude (~ 4 hPa), and 5–10 pptv at pressures ≤ 0.5 hPa for daytime mid-latitude conditions. For nighttime measurements, a systematic error of 8 pptv was estimated for the ClO peak altitude (~ 2 hPa). The SMILES NICT v2.1.5 ClO profiles agree with those derived from another level-2 processor developed by the Japan Aerospace Exploration Agency (JAXA) within the bias uncertainties, except for the nighttime measurements in the low and middle latitude regions where the SMILES NICT v2.1.5 profiles have a negative bias of ~ 30 pptv in the lower stratosphere. This bias is considered to be due to the use of a limited spectral bandwidth in the retrieval process of SMILES NICT v2.1.5, which makes it difficult to distinguish between the weak ClO signal and wing contributions of spectral features outside the bandwidth. In the middle and upper stratosphere outside the polar regions, no significant systematic bias was found for the SMILES NICT ClO profile with respect to data sets from other instruments such as the Aura Microwave Limb Sounder (MLS), the Odin Sub-Millimetre Radiometer (SMR), the Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), and the ground-based radiometer at Mauna Kea, which demonstrates the scientific usability of the SMILES ClO data including the diurnal variations. Inside the chlorine-activated polar vortex, the SMILES NICT v2.1.5 ClO profiles show larger volume mixing ratios by 0.4 ppbv (30%) at 50 hPa compared to those of the JAXA processed profiles. This discrepancy is also considered to be an effect of the limited spectral bandwidth in the retrieval processing. We also compared the SMILES NICT ClO profiles of chlorine-activated polar vortex conditions with those measured by the balloon-borne instruments: Terahertz and submillimeter Limb Sounder (TELIS) and the MIPAS-balloon instrument (MIPAS-B). In conclusion, the SMILES NICT v2.1.5 ClO data can be used at pressures ≤ ~30 hPa for scientific analysis.

Description: Trajectory matching of ozonesondes and MOZAIC measurements in the UTLS – Part 1: Method description and application at Payerne, Switzerland Atmospheric Measurement Techniques, 6, 3393-3406, 2013 Author(s): J. Staufer, J. Staehelin, R. Stübi, T. Peter, F. Tummon, and V. Thouret With the aim of improving ozonesonde observations in the upper troposphere/lower stratosphere (UTLS), we use three-dimensional forward and backward trajectories, driven by ERA-Interim wind fields to match and compare ozonesonde measurements at Payerne (Switzerland) with observations from the MOZAIC aircraft program from 1994–2009. The uncertainties associated with the sonde–MOZAIC match technique were assessed using "self-matches", i.e. matches of instruments of the same type, such as MOZAIC–MOZAIC. Despite strong vertical gradients of ozone at the tropopause, which render the match approach difficult, the method provides excellent results, showing mean differences between different MOZAIC aircraft of ±2% (typically with a few hours between the up- and downstream match points). Matches between MOZAIC aircraft and Payerne ozonesondes show an agreement of ±5% for sondes equipped with electrochemical concentration cells (ECC) and between 〈 5% (not scaled to total ozone) and 〈 10% (scaled) for the Brewer–Mast (BM) sondes after 1998. Prior to 1998, BM sondes show an offset of around 20% (scaled). No break can be identified through the change from the BM to ECC sonde types in September 2002. A comparison of BM sondes with ozone measurements from the NOXAR B747 project for the period 1995–1996 show a smaller offset of around 15% (scaled), which may indicate a small drift in the MOZAIC calibration.

Description: COMPASS – COMparative Particle formation in the Atmosphere using portable Simulation chamber Study techniques Atmospheric Measurement Techniques, 6, 3407-3423, 2013 Author(s): B. Bonn, S. Sun, W. Haunold, R. Sitals, E. van Beesel, L. dos Santos, B. Nillius, and S. Jacobi In this study we report the set-up of a novel twin chamber technique that uses the comparative method and establishes an appropriate connection of atmospheric and laboratory methods to broaden the tools for investigations. It is designed to study the impact of certain parameters and gases on ambient processes, such as particle formation online, and can be applied in a large variety of conditions. The characterisation of both chambers proved that both chambers operate identically, with a residence time x T (COMPASS1) = 26.5 ± 0.3 min and x T (COMPASS2) = 26.6 ± 0.4 min, at a typical flow rate of 15 L min −1 and a gas leak rate of (1.6 ± 0.8) × 10 −5 s −1 . Particle loss rates were found to be larger (due to the particles' stickiness to the chamber walls), with an extrapolated maximum of 1.8 × 10 −3 s −1 at 1 nm, i.e. a hundredfold of the gas leak rate. This latter value is associated with sticky non-volatile gaseous compounds, too. Comparison measurement showed no significant differences. Therefore operation under atmospheric conditions is trustworthy. To indicate the applicability and the benefit of the system, a set of experiments was conducted under different conditions, i.e. urban and remote, enhanced ozone and terpenes as well as reduced sunlight. In order to do so, an ozone lamp was applied to enhance ozone in one of two chambers; the measurement chamber was protected from radiation by a first-aid cover and volatile organic compounds (VOCs) were added using a small additional flow and a temperature-controlled oven. During the elevated ozone period, ambient particle number and volume increased substantially at urban and remote conditions, but by a different intensity. Protection of solar radiation displayed a clear negative effect on particle number, while terpene addition did cause a distinct daily pattern. E.g. adding β pinene particle number concentration rose by 13% maximum at noontime, while no significant effect was observable during darkness. Therefore, the system is a useful tool for investigating local precursors and the details of ambient particle formation at surface locations as well as potential future feedback processes.

Description: Cloud discrimination in probability density functions of limb-scattered sunlight measurements Atmospheric Measurement Techniques, 6, 3359-3368, 2013 Author(s): E. N. Normand, J. T. Wiensz, A. E. Bourassa, and D. A. Degenstein A technique characterizing the distribution of cirrus cloud-top occurrences from the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb-scattering radiance profiles is presented. The technique involves computing scattering residual profiles by comparing normalized measured radiance and modelled molecular radiance profiles where enhancements in the measured radiance indicate the presence of clouds. Probability density functions of scattering residuals show the distribution is not a continuum measurement; there is a distinction between the cloudy and cloud-free conditions. Observations show high cloud-top occurrences in the upper troposphere and lower stratosphere region above Indonesia and Central America. Results obtained using this technique with OSIRIS measurements are compared to those obtained by Sassen et al. (2008) with Cloud-Aerosol Lidar Pathfinder Satellite Observations (CALIPSO) nadir measurements and to those obtained by Wang et al. (1996) with Stratospheric Aerosol and Gas Experiment (SAGE) II solar occultation measurements.

Description: Autofluorescence of atmospheric bioaerosols: spectral fingerprints and taxonomic trends of pollen Atmospheric Measurement Techniques, 6, 3369-3392, 2013 Author(s): C. Pöhlker, J. A. Huffman, J.-D. Förster, and U. Pöschl Primary biological aerosol particles (PBAP) are important factors in atmospheric cycling, climate, and public health. Pollen is a major fraction of PBAP and is receiving increasing attention due to its high allergenic potential and the associated impacts on personal life quality and economy. Recently, autofluorescence-based techniques have proven to be valuable tools for real time, in situ quantification and classification of PBAP. First studies suggest that the autofluorescence of pollen may be sufficiently selective to be utilized for an automated and real-time monitoring of pollen in ambient air. However, the degree of selectivity autofluorescence can provide is still in question and actively debated. This study addresses the origin, properties, and selectivity of autofluorescence from natural pollen by fluorescence microscopy and spectroscopy measurements along with a systematic synthesis of related literature. We show that dry pollen reveals characteristic and reproducible autofluorescence signatures which are shaped by cell wall associated fluorophores, such as phenolic compounds and carotenoid pigments. In addition, fluorescence signals from proteins and chlorophyll a were observed in some species. The abundance and intensity of the individual fluorescence signals show certain taxonomic trends and allow systematic differentiation from bacteria and fungal spores due to the lack of proteins on the grain surface. Principal component analysis was used to explore the discrimination potential of pollen autofluorescence, in combination with size and shape, revealing a differentiation of pollen on family level. Our results help explore the levels of selectivity that autofluorescence-based techniques can provide to PBAP analysis and will support the development and application of autofluorescence-based detectors for monitoring of allergenic pollen in the atmosphere.

Description: 0.355-micrometer direct detection wind lidar under testing during a field campaign in consideration of ESA's ADM-Aeolus mission Atmospheric Measurement Techniques, 6, 3349-3358, 2013 Author(s): S. Lolli, A. Delaval, C. Loth, A. Garnier, and P. H. Flamant The atmospheric wind field information is a key issue to numerical weather prediction (NWP) and climate studies. The Atmospheric Dynamic Mission-Aeolus is currently developed by the European Space Agency (ESA) to launch a wind sensing Doppler lidar in mid-2015. The high spectral resolution lidar concept is using backscattered laser signals from molecules and particles to provide accurate horizontal wind velocity measurements in the depth of atmosphere. The Aeolus lidar, so-called ALADIN, will operate in UV at 0.355 μm. The combination of air molecules and UV laser light is intended to provide wind data evenly distributed everywhere in the lower atmosphere (below 30 km altitude). The goal of the ESA's Aeolus mission is to enhance the present meteorological observations system over sparse wind data regions, and more importantly to provide direct wind information in the tropics where no geostrophic wind can be derived from mass fields obtained from passive radiometer satellite. The 0.355 μm lidar concept was under testing during a field campaign conducted at the Haute-Provence Observatory, France, in 1999. Several active remote sensors were deployed on the site, and it was the opportunity to address the self-consistency of wind measurements made by different lidars, a 72 MHz radar, and conventional balloon radio soundings. The paper presents the comparison of different remote sensors using two criteria: Pearson cross-correlation coefficient and root mean square error. The methodology discussed here may be useful in future ESA Aeolus validation campaigns involving different kinds of instruments.

Description: Reporting the sensitivity of laser-induced fluorescence instruments used for HO 2 detection to an interference from RO 2 radicals and introducing a novel approach that enables HO 2 and certain RO 2 types to be selectively measured Atmospheric Measurement Techniques, 6, 3425-3440, 2013 Author(s): L. K. Whalley, M. A. Blitz, M. Desservettaz, P. W. Seakins, and D. E. Heard Laboratory studies have revealed that alkene-derived RO 2 and longer chain alkane-derived RO 2 (〉 C 3 ) radicals rapidly convert to HO 2 and then to OH in the presence of NO in a fluorescence assay by gas expansion (FAGE) detection cell (Fuchs et al., 2011). Three different FAGE cells that have been used to make ambient measurements of OH and HO 2 in the University of Leeds ground-based instrument have been assessed to determine the sensitivity of each cell, when operating in HO 2 detection mode, to RO 2 radicals. The sensitivity to this interference was found to be highly dependent on cell design and operating parameters. Under the operating conditions employed, during fieldwork undertaken in the Borneo rainforest in 2008, an OH yield of 17% was experimentally determined for both ethene- and isoprene-derived RO 2 radicals. The high pumping capacity of this system, resulting in a short residence time in the cell, coupled with poor mixing of NO into the ambient air-stream for the titration of HO 2 to OH effectively minimised this potential interference. An OH yield of 46% was observed for ethene-derived RO 2 radicals when a smaller detection cell was used, in which the mixing of NO into the ambient air was improved and the cell residence times were much longer. For a newly developed RO x LIF cell, used for detection of HO 2 and RO 2 radicals an OH yield of 95% was observed for ethene-derived RO 2 radicals, when running in HO 2 mode. In experiments in which conditions ensured the conversion of RO 2 to OH were complete, the yields of OH from a range of different RO 2 species agreed well with model predictions based on the Master Chemical Mechanism version 3.2. For ethene and isoprene-derived RO 2 species, the relative sensitivity of FAGE was found to be close to that for HO 2 , with an OH yield of 100% and 92%, respectively. For the longer chain or cyclic alkane-derived RO 2 radicals (〉 C 3 ), model predicted OH yields were highly dependent upon temperature. A model predicted OH yield of 74% at 298 K and 36% at 255 K were calculated for cyclohexane-derived RO 2 radicals, and an experimental yield of 38% was observed indicating that the temperature within the cell was below ambient owing to the supersonic expansion of the airstream in the low pressure cell. These findings suggest that observations of HO 2 by some LIF instruments worldwide may be higher than the true value if the instruments were sensitive to these RO 2 species. If this is the case, it becomes necessary to compare atmospheric chemistry model simulations to HO 2 * observations, where HO 2 * = [HO 2 ] + Σ i α i [RO 2 i ], and α i is the mean fractional contribution of the RO 2 species that interfere (RO 2 i ). This methodology, however, relies on model simulations of speciated RO 2 radicals, as instrumentation to make speciated RO 2 measurements does not currently exist. Here we present an approach that enables the concentration of HO 2 and RO 2 i to be selectively determined by varying the concentration of NO injected into a FAGE cell. Measurements of [HO 2 ] and [RO 2 i ] taken in London are presented.

Description: Characterization of the planetary boundary layer height and structure by Raman lidar: comparison of different approaches Atmospheric Measurement Techniques, 6, 3515-3525, 2013 Author(s): D. Summa, P. Di Girolamo, D. Stelitano, and M. Cacciani The planetary boundary layer (PBL) includes the portion of the atmosphere which is directly influenced by the presence of the earth's surface. Aerosol particles trapped within the PBL can be used as tracers to study the boundary-layer vertical structure and time variability. As a result of this, elastic backscatter signals collected by lidar systems can be used to determine the height and the internal structure of the PBL. The present analysis considers three different methods to estimate the PBL height. The first method is based on the determination of the first-order derivative of the logarithm of the range-corrected elastic lidar signals. Estimates of the PBL height for specific case studies obtained through this approach are compared with simultaneous estimates from the potential temperature profiles measured by radiosondes launched simultaneously to lidar operation. Additional estimates of the boundary layer height are based on the determination of the first-order derivative of the range-corrected rotational Raman lidar signals. This latter approach results to be successfully applicable also in the afternoon–evening decaying phase of the PBL, when the effectiveness of the approach based on the elastic lidar signals may be compromised or altered by the presence of the residual layer. Results from these different approaches are compared and discussed in the paper, with a specific focus on selected case studies collected by the University of Basilicata Raman lidar system BASIL during the Convective and Orographically-induced Precipitation Study (COPS).

Description: Photoacoustic and nephelometric spectroscopy of aerosol optical properties with a supercontinuum light source Atmospheric Measurement Techniques, 6, 3501-3513, 2013 Author(s): N. Sharma, I. J. Arnold, H. Moosmüller, W. P. Arnott, and C. Mazzoleni A novel multi-wavelength photoacoustic-nephelometer spectrometer (SC-PNS) has been developed for the optical characterization of atmospheric aerosol particles. This instrument integrates a white light supercontinuum laser with photoacoustic and nephelometric spectroscopy to measure aerosol absorption and scattering coefficients at five wavelength bands (centered at 417, 475, 542, 607, and 675 nm). These wavelength bands are selected from the continuous spectrum of the laser (ranging from 400–2200 nm) using a set of optical interference filters. Absorption and scattering measurements on laboratory-generated aerosol samples were performed sequentially at each wavelength band. To test the instrument we measured the wavelength dependence of absorption and scattering coefficients of kerosene soot and common salt aerosols. Results were favorably compared to those obtained with a commercial 3-wavelength photoacoustic and nephelometer instrument demonstrating the utility of the SC light source for studies of aerosol optical properties at selected wavelengths. Here, we discuss instrument design, development, calibration, performance and experimental results.

Description: Carbon Monitoring Satellite (CarbonSat): assessment of atmospheric CO 2 and CH 4 retrieval errors by error parameterization Atmospheric Measurement Techniques, 6, 3477-3500, 2013 Author(s): M. Buchwitz, M. Reuter, H. Bovensmann, D. Pillai, J. Heymann, O. Schneising, V. Rozanov, T. Krings, J. P. Burrows, H. Boesch, C. Gerbig, Y. Meijer, and A. Löscher Carbon Monitoring Satellite (CarbonSat) is one of two candidate missions for ESA's Earth Explorer 8 (EE8) satellite to be launched around the end of this decade. The overarching objective of the CarbonSat mission is to improve our understanding of natural and anthropogenic sources and sinks of the two most important anthropogenic greenhouse gases (GHGs) carbon dioxide (CO 2 ) and methane (CH 4 ). The unique feature of CarbonSat is its "GHG imaging capability", which is achieved via a combination of high spatial resolution (2 km × 2 km) and good spatial coverage (wide swath and gap-free across- and along-track ground sampling). This capability enables global imaging of localized strong emission source, such as cities, power plants, methane seeps, landfills and volcanos, and likely enables better disentangling of natural and anthropogenic GHG sources and sinks. Source–sink information can be derived from the retrieved atmospheric column-averaged mole fractions of CO 2 and CH 4 , i.e. X CO 2 and X CH 4 , by inverse modelling. Using the most recent instrument and mission specification, an error analysis has been performed using the Bremen optimal EStimation DOAS (BESD/C) retrieval algorithm. We assess the retrieval performance for atmospheres containing aerosols and thin cirrus clouds, assuming that the retrieval forward model is able to describe adequately all relevant scattering properties of the atmosphere. To compute the errors for each single CarbonSat observation in a one-year period, we have developed an error parameterization scheme comprising six relevant input parameters: solar zenith angle, surface albedo in two bands, aerosol and cirrus optical depth, and cirrus altitude variations. Other errors, e.g. errors resulting from aerosol type variations, are partially quantified but not yet accounted for in the error parameterization. Using this approach, we have generated and analysed one year of simulated CarbonSat observations. Using this data set we estimate that systematic errors are for the overwhelming majority of cases (≈ 85%) below 0.3 ppm for X CO 2 (below 0.5 ppm for 99.5%) and below 2 ppb for X CH 4 (below 4 ppb for 99.3%). We also show that the single-measurement precision is typically around 1.2 ppm for X CO 2 and 7 ppb for X CH 4 (1σ). The number of quality-filtered observations over cloud- and ice-free land surfaces is in the range of 33 to 47 million per month depending on season. Recently it has been shown that terrestrial vegetation chlorophyll fluorescence (VCF) emission needs to be considered for accurate X CO 2 retrieval. We therefore retrieve VCF from clear Fraunhofer lines located around 755 nm and show that CarbonSat will provide valuable information on VCF. We estimate that the VCF single-measurement precision is approximately 0.3 mW m −2 nm −1 sr −1 (1σ).

Description: A method for sizing submicrometer particles in air collected on Formvar films and imaged by scanning electron microscope Atmospheric Measurement Techniques, 6, 3459-3475, 2013 Author(s): E. Hamacher-Barth, K. Jansson, and C. Leck A method was developed to systematically investigate individual aerosol particles collected onto a polyvinyl formal (Formvar)-coated copper grid with scanning electron microscopy. At very mild conditions with a low accelerating voltage of 2 kV and Gentle Beam mode aerosol particles down to 20 nm in diameter can be observed. Subsequent processing of the images with digital image analysis provides size resolved and morphological information (elongation, circularity) on the aerosol particle population. Polystyrene nanospheres in the expected size range of the ambient aerosol particles (20–900 nm in diameter) were used to confirm the accuracy of sizing and determination of morphological parameters. The relative standard deviation of the diameters of the spheres was better than ±10% for sizes larger than 40 nm and ±18% for 21 nm particles compared to the manufacturer's certificate. Atmospheric particles were collected during an icebreaker expedition to the high Arctic (north of 80°) in the summer of 2008. Two samples collected during two different meteorological regimes were analyzed. Their size distributions were compared with simultaneously collected size distributions from a Twin Differential Mobility Particle Sizer, which confirmed that a representative fraction of the aerosol particles was imaged under the electron microscope. The size distributions obtained by scanning electron microscopy showed good agreement with the Twin Differential Mobility Sizer in the Aitken mode, whereas in the accumulation mode the size determination was critically dependent on the contrast of the aerosol with the Formvar-coated copper grid. The morphological properties (elongation, circularity) changed with the number of days the air masses spent over the pack-ice area north of 80° before the aerosol particles were collected at the position of the icebreaker and are thus an appropriate measure to characterize transformation processes of ambient aerosol particles.

Description: Assessing remote polarimetric measurement sensitivities to aerosol emissions using the geos-chem adjoint model Atmospheric Measurement Techniques, 6, 3441-3457, 2013 Author(s): B. S. Meland, X. Xu, D. K. Henze, and J. Wang Uncertainties in aerosol sources, microphysical properties, and global distributions undermine efforts to evaluate the radiative impacts of atmospheric aerosols. In this work, we investigate the feasibility of using remote polarimetric measurements for constraining aerosol and aerosol precursor emissions in light of these uncertainties. A model that incorporates a radiative transfer model with forward and adjoint chemical transport models has been applied to quantify the sensitivity of the reflectance at the top of atmosphere over land to aerosol emissions and microphysical properties. A set of simulated satellite observations, one intensity based and one capable of polarimetric measurements, are used to illustrate differences in the assimilation potential between the two. It is found that the sensitivity of the polarized reflectance to aerosol and aerosol precursor emissions tends to be significantly higher than that of the intensity for cases of non-absorbing aerosols. This is true even when the polarimetric sampling scheme is spatially sparser than that of the intensity sampling. This framework allows us to quantify upper limits on the uncertainties in the aerosol microphysical properties for which a 50% change in aerosol emissions is detectable using these simulated observations. It was found that although typical current remote sensing instrumentation provides retrievals of the refractive index and effective radius with accuracies within acceptable limits to detect a 50% change in emissions, retrievals of the effective variance contain uncertainties too large to detect these changes in emissions. These results may guide new applications of polarimetric measurements to constrain aerosol sources, and thus reduce uncertainty in our broader understanding of the impacts of aerosols on climate.

Description: Retrieval of desert dust aerosol vertical profiles from IASI measurements in the TIR atmospheric window Atmospheric Measurement Techniques, 6, 2577-2591, 2013 Author(s): S. Vandenbussche, S. Kochenova, A. C. Vandaele, N. Kumps, and M. De Mazière Desert dust aerosols are the most prominent tropospheric aerosols, playing an important role in the earth's climate. However, their radiative forcing is currently not known with sufficient precision to even determine its sign. The sources of uncertainty are multiple, one of them being a poor characterisation of the dust aerosol's vertical profile on a global scale. In this work, we tackle this scientific issue by designing a method for retrieving dust aerosol vertical profiles from Thermal Infrared measurements by Infrared Atmospheric Sounding Interferometer (IASI) instruments onboard the Metop satellite series. IASI offers almost global coverage twice a day, and long (past and future) time series of radiances, therefore being extremely well suited for climate studies. Our retrieval follows Rodger's formalism and is based on a two-step approach, treating separately the issues of low altitude sensitivity and difficult a priori definition. We compare our results for a selected test case above the Atlantic Ocean and North Africa in June 2009, with optical depth data from MODIS, aerosol absorbing index from GOME-2 and OMI, and vertical profiles of extinction coefficients from CALIOP. We also use literature information on desert dust sources to interpret our results above land. Our retrievals provide perfectly reasonable results in terms of optical depth. The retrieved vertical profiles (with on average 1.5 degrees of freedom) show most of the time sensitivity down to the lowest layer, and agree well with CALIOP extinction profiles for medium to high dust optical depth. We conclude that this new method is extremely promising for improving the scientific knowledge about the 3-D distribution of desert dust aerosols in the atmosphere.

Description: Nabro volcano aerosol in the stratosphere over Georgia, South Caucasus from ground-based spectrometry of twilight sky brightness Atmospheric Measurement Techniques, 6, 2563-2576, 2013 Author(s): N. Mateshvili, D. Fussen, G. Mateshvili, I. Mateshvili, F. Vanhellemont, E. Kyrölä, S. Tukiainen, J. Kujanpää, C. Bingen, C. Robert, C. Tétard, and E. Dekemper Ground-based spectral measurements of twilight sky brightness were carried out between September 2009 and August 2011 in Georgia, South Caucasus. The algorithm which allowed to retrieve the lower stratospheric and upper tropospheric aerosol extinction profiles was developed. The Monte-Carlo technique was used to correctly represent multiple scattering in a spherical atmosphere. The estimated stratospheric aerosol optical depths at a wavelength of 780 nm were: 6 × 10 −3 ± 2 × 10 −3 (31 August 2009–29 November 2009), 2.5 × 10 −3 ± 7 × 10 −4 (20 March 2010–15 January 2011) and 8 × 10 −3 ± 3 × 10 −3 (18 July 2011–3 August 2011). The optical depth values correspond to the moderately elevated stratospheric aerosol level after the Sarychev eruption in 2009, background stratospheric aerosol layer, and the volcanically disturbed stratospheric aerosol layer after the Nabro eruption in June 2011.

Description: New retrieval of BrO from SCIAMACHY limb: an estimate of the stratospheric bromine loading during April 2008 Atmospheric Measurement Techniques, 6, 2549-2561, 2013 Author(s): J. P. Parrella, K. Chance, R. J. Salawitch, T. Canty, M. Dorf, and K. Pfeilsticker We present a new retrieval of stratospheric BrO (bromine monoxide) from channel 2 SCIAMACHY (SCanning Imaging Absorption spectrometer for Atmospheric CHartographY) limb observations. Retrievals are shown to agree with independent balloon observations to within one standard deviation of the retrieval noise. We retrieve BrO profiles for all of April 2008, and apply simulated [BrO]/[Br y ] (bromine monoxide : stratospheric inorganic bromine) ratios to estimate the stratospheric Br y loading. We find 23.5 ± 6 ppt Br, suggesting 7 ppt Br from short-lived bromocarbons to be at the high end of the current best estimate (3–8 ppt). The 6 ppt Br uncertainty estimate is dominated by the 21% uncertainty in the simulated [BrO] / [Br y ] ratio due to propagation of errors from the underlying chemical kinetics.

Description: Solar Backscatter UV (SBUV) total ozone and profile algorithm Atmospheric Measurement Techniques, 6, 2533-2548, 2013 Author(s): P. K. Bhartia, R. D. McPeters, L. E. Flynn, S. Taylor, N. A. Kramarova, S. Frith, B. Fisher, and M. DeLand We describe the algorithm that has been applied to develop a 42 yr record of total ozone and ozone profiles from eight Solar Backscatter UV (SBUV) instruments launched on NASA and NOAA satellites since April 1970. The Version 8 (V8) algorithm was released more than a decade ago and has been in use since then at NOAA to produce their operational ozone products. The current algorithm (V8.6) is basically the same as V8, except for updates to instrument calibration, incorporation of new ozone absorption cross-sections, and new ozone and cloud height climatologies. Since the V8 algorithm has been optimized for deriving monthly zonal mean (MZM) anomalies for ozone assessment and model comparisons, our emphasis in this paper is primarily on characterizing the sources of errors that are relevant for such studies. When data are analyzed this way the effect of some errors, such as vertical smoothing of short-term variability, and noise due to clouds and aerosols diminish in importance, while the importance of others, such as errors due to vertical smoothing of the quasi-biennial oscillation (QBO) and other periodic and aperiodic variations, become more important. With V8.6 zonal mean data we now provide smoothing kernels that can be used to compare anomalies in SBUV profile and partial ozone columns with models. In this paper we show how to use these kernels to compare SBUV data with Microwave Limb Sounder (MLS) ozone profiles. These kernels are particularly useful for comparisons in the lower stratosphere where SBUV profiles have poor vertical resolution but partial column ozone values have high accuracy. We also provide our best estimate of the smoothing errors associated with SBUV MZM profiles. Since smoothing errors are the largest source of uncertainty in these profiles, they can be treated as error bars in deriving interannual variability and trends using SBUV data and for comparing with other measurements. In the V8 and V8.6 algorithms we derive total column ozone by integrating the SBUV profiles, rather than from a separate set of wavelengths, as was done in previous algorithm versions. This allows us to extend the total ozone retrieval to 88° solar zenith angle (SZA). Since the quality of total column data is affected by reduced sensitivity to ozone in the lower atmosphere by cloud and Rayleigh attenuation, which gets worse with increasing SZA, we provide our best estimate of these errors, as well as the kernels that can be used to test the sensitivity of the derived columns to long-term changes in ozone in the lower atmosphere.

Description: Measurement of the Arctic UTLS composition in presence of clouds using millimetre-wave heterodyne spectroscopy Atmospheric Measurement Techniques, 6, 2683-2701, 2013 Author(s): E. Castelli, B. M. Dinelli, S. Del Bianco, D. Gerber, B. P. Moyna, R. Siddans, B. J. Kerridge, and U. Cortesi MARSCHALS (Millimetre-wave Airborne Receivers for Spectroscopic CHaracterisation in Atmospheric Limb Sounding) is a limb viewing instrument working in the millimetre and sub-millimetre spectral regions (from 294 to 349 GHz). The scientific rationale of MARSCHALS is the study of the Upper Troposphere and Lower Stratosphere region. In March 2010 MARSCHALS was deployed on-board the M-55 Geophysica stratospheric aircraft during the PREMIER(PRocess Exploration through Measurements of Infrared and millimetre-wave Emitted Radiation)-Ex field campaign. From the campaign base at Kiruna, Sweden, a research flight to investigate the Arctic atmosphere was conducted. For the first time the instrument fully exploited the three spectral bands. In this paper, we present results of the analysis of MARSCHALS measurements acquired during the PREMIER-Ex flight as processed by the Millimetre-wave Atmospheric Retrieval Code. For the second time after the SCOUT-O3 flight in 2005, MARSCHALS measured vertical distributions of temperature, water vapour, ozone and nitric acid over an altitude range of 4 to 24 km. In addition, vertical profiles of carbon monoxide and nitrous oxide were obtained for the first time. The measurements were performed in clear sky conditions and in presence of low and high altitude clouds (that were able to obscure measurements in the middle infrared spectroscopic region) and some information about thick clouds were extracted from the data. The capabilities to derive information on upper tropospheric and lower stratospheric vertical profiles of temperature and minor constituents from millimetre-wave limb sounding observations in the northern polar region are presented and discussed for each of the individual targets. The results of MARSCHALS data analysis contributed to demonstrate the scientific relevance and technical feasibility of millimetre-wave limb-sounding of the UTLS proposed for the ESA Earth Explorer 7 candidate Core Mission PREMIER. PREMIER was not selected at the end of the Earth Explorer 7 evaluation process, but it is still being considered for future launch opportunities.

Description: A feasibility study for the retrieval of the total column precipitable water vapour from satellite observations in the blue spectral range Atmospheric Measurement Techniques, 6, 2593-2605, 2013 Author(s): T. Wagner, S. Beirle, H. Sihler, and K. Mies We present a new algorithm for satellite retrievals of the atmospheric water vapour column in the blue spectral range. The water vapour absorption cross section in the blue spectral range is much weaker than in the red spectral range. Thus the detection limit and the uncertainty of individual observations are systematically larger than for retrievals at longer wavelengths. Nevertheless, water vapour retrievals in the blue spectral range have also several advantages: since the surface albedo in the blue spectral range is similar over land and ocean, water vapour retrievals are more consistent than for longer wavelengths. Compared to retrievals at longer wavelengths, the sensitivity for atmospheric layers close to the surface is higher due to the (typically 2 to 3 times) higher ocean albedo in the blue. Water vapour retrievals in the blue spectral range are also possible for satellite sensors, which do not measure at longer wavelengths of the visible spectral range like the Ozone Monitoring Instrument (OMI). We investigated details of the water vapour retrieval in the blue spectral range based on radiative transfer simulations and observations from the Global Ozone Monitoring Experiment 2 (GOME-2) and OMI. It is demonstrated that it is possible to retrieve the atmospheric water vapour column density in the blue spectral range over most parts of the globe. The findings of our study are of importance also for future satellite missions (e.g. Sentinel 4 and 5).

Description: A fast method for the retrieval of integrated longwave and shortwave top-of-atmosphere upwelling irradiances from MSG/SEVIRI (RRUMS) Atmospheric Measurement Techniques, 6, 2627-2640, 2013 Author(s): M. Vázquez-Navarro, B. Mayer, and H. Mannstein A new Rapid Retrieval of Upwelling irradiances from MSG/SEVIRI (RRUMS) is presented. It has been developed to observe the top-of-atmosphere irradiances of small scale and rapidly changing features that are not sufficiently resolved by specific Earth radiation budget sensors. Our retrieval takes advantage of the spatial and temporal resolution of MSG/SEVIRI and provides outgoing longwave and reflected shortwave radiation only by means of a combination of SEVIRI channels. The longwave retrieval is based on a simple linear combination of brightness temperatures from the SEVIRI infrared channels. The shortwave retrieval is based on a neural network that requires as input the visible and near-infrared SEVIRI channels. Both LW and SW algorithms have been validated by comparing their results with CERES and GERB irradiance observations. While being less accurate than their dedicated counterparts, the SEVIRI-based methods have two major advantages compared to CERES and GERB: their higher spatial resolution and the better temporal resolution. With our retrievals it is possible to observe the radiative effect of small-scale features such as cumulus clouds, cirrus clouds, or aircraft contrails. The spatial resolution of SEVIRI is 3 km × 3 km in the sub-satellite point, remarkably better than that of CERES (20 km) or GERB (45 km). The temporal resolution is 15 min (5 min in the Rapid-Scan mode), the same as GERB, but significantly better than that of CERES which, being on board of a polar orbiting satellite, has a temporal resolution as low as 2 overpasses per day.

Description: A threshold-based cloud mask for the high-resolution visible channel of Meteosat Second Generation SEVIRI Atmospheric Measurement Techniques, 6, 2713-2723, 2013 Author(s): S. Bley and H. Deneke A threshold-based cloud mask for the high-resolution visible (HRV) channel (1 × 1 km 2 ) of the Meteosat SEVIRI (Spinning Enhanced Visible and Infrared Imager) instrument is introduced and evaluated. It is based on operational EUMETSAT cloud mask for the low-resolution channels of SEVIRI (3 × 3 km 2 ), which is used for the selection of suitable thresholds to ensure consistency with its results. The aim of using the HRV channel is to resolve small-scale cloud structures that cannot be detected by the low-resolution channels. We find that it is of advantage to apply thresholds relative to clear-sky reflectance composites, and to adapt the threshold regionally. Furthermore, the accuracy of the different spectral channels for thresholding and the suitability of the HRV channel are investigated for cloud detection. The case studies show different situations to demonstrate the behavior for various surface and cloud conditions. Overall, between 4 and 24% of cloudy low-resolution SEVIRI pixels are found to contain broken clouds in our test data set depending on considered region. Most of these broken pixels are classified as cloudy by EUMETSAT's cloud mask, which will likely result in an overestimate if the mask is used as an estimate of cloud fraction. The HRV cloud mask aims for small-scale convective sub-pixel clouds that are missed by the EUMETSAT cloud mask. The major limit of the HRV cloud mask is the minimum cloud optical thickness (COT) that can be detected. This threshold COT was found to be about 0.8 over ocean and 2 over land and is highly related to the albedo of the underlying surface.

Description: Retrieval of aerosol parameters from the oxygen A band in the presence of chlorophyll fluorescence Atmospheric Measurement Techniques, 6, 2725-2740, 2013 Author(s): A. F. J. Sanders and J. F. de Haan We have investigated the precision of retrieved aerosol parameters for a generic aerosol retrieval algorithm over vegetated land using the O 2 A band. Chlorophyll fluorescence is taken into account in the forward model. Fluorescence emissions are modeled as isotropic contributions to the upwelling radiance field at the surface and they are retrieved along with aerosol parameters. Precision is calculated by propagating measurement errors and a priori errors, including model parameter errors, using the forward model's derivatives. Measurement errors consist of noise and calibration errors. The model parameter errors considered are related to the single scattering albedo, surface pressure and temperature profile. We assume that measurement noise is dominated by shot noise; thus, results apply to grating spectrometers in particular. We describe precision for various atmospheric states, observation geometries and spectral resolutions of the instrument in a number of retrieval simulations. These precision levels can be compared with user requirements. A comparison of precision estimates with the literature and an analysis of the dependence on the a priori error in the fluorescence emission indicate that aerosol parameters can be retrieved in the presence of chlorophyll fluorescence: if fluorescence is present, fluorescence emissions should be included in the state vector to avoid biases in retrieved aerosol parameters.

Description: Online determination of levoglucosan in ambient aerosols with particle-into-liquid sampler – high-performance anion-exchange chromatography – mass spectrometry (PILS–HPAEC–MS) Atmospheric Measurement Techniques, 6, 2839-2849, 2013 Author(s): K. Saarnio, K. Teinilä, S. Saarikoski, S. Carbone, S. Gilardoni, H. Timonen, M. Aurela, and R. Hillamo Biomass burning, such as domestic heating, agricultural, and wild open-land fires, has a significant influence on the atmosphere at the global and, especially, at the local scale. Levoglucosan has been shown to be a good tracer for biomass burning emissions in atmospheric particulate matter, and several analytical techniques have been presented for the determination of levoglucosan from filter samples. In this paper, a novel combination of a particle-into-liquid sampler (PILS) to a high-performance anion-exchange chromatograph (HPAEC) with the detection by a mass spectrometer (MS) is presented for the online analysis of levoglucosan in ambient particles. The PILS–HPAEC–MS technique enables a fast online analysis of levoglucosan from the particulate samples. The method was tested at an urban background station in Helsinki, Finland, in winter 2011. A comparison with simultaneous levoglucosan measurements from filter samples by the HPAEC–MS was performed and it showed a good agreement between the online and offline methods. Additionally, the online levoglucosan data were compared with the biomass burning tracer fragments measured by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). As there were no local biomass burning sources close to the measurement station, online levoglucosan measurements revealed that most of the particles from biomass burning were either regionally distributed or long-range transported in the urban background of Helsinki. The average levoglucosan concentrations were relatively low (average 0.083 μg m −3 ) during the measurement campaign. The highest concentration peak measured for levoglucosan (1.4 μg m −3 ) seemed to originate from biomass burning in the Baltic countries, likely in Estonia, that was transported to Helsinki.

Description: Error budget analysis of SCIAMACHY limb ozone profile retrievals using the SCIATRAN model Atmospheric Measurement Techniques, 6, 2825-2837, 2013 Author(s): N. Rahpoe, C. von Savigny, M. Weber, A.V. Rozanov, H. Bovensmann, and J. P. Burrows A comprehensive error characterization of SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric CHartographY) limb ozone profiles has been established based upon SCIATRAN transfer model simulations. The study was carried out in order to evaluate the possible impact of parameter uncertainties, e.g. in albedo, stratospheric aerosol optical extinction, temperature, pressure, pointing, and ozone absorption cross section on the limb ozone retrieval. Together with the a posteriori covariance matrix available from the retrieval, total random and systematic errors are defined for SCIAMACHY ozone profiles. Main error sources are the pointing errors, errors in the knowledge of stratospheric aerosol parameters, and cloud interference. Systematic errors are of the order of 7%, while the random error amounts to 10–15% for most of the stratosphere. These numbers can be used for the interpretation of instrument intercomparison and validation of the SCIAMACHY V 2.5 limb ozone profiles in a rigorous manner.

Description: Retrieval of aerosol single-scattering albedo and polarized phase function from polarized sun-photometer measurements for Zanjan's atmosphere Atmospheric Measurement Techniques, 6, 2659-2669, 2013 Author(s): A. Bayat, H. R. Khalesifard, and A. Masoumi The polarized phase function of atmospheric aerosols has been investigated for the atmosphere of Zanjan, a city in northwest Iran. To do this, aerosol optical depth, Ångström exponent, single-scattering albedo, and polarized phase function have been retrieved from the measurements of a Cimel CE 318-2 polarized sun-photometer from February 2010 to December 2012. The results show that the maximum value of aerosol polarized phase function as well as the polarized phase function retrieved for a specific scattering angle (i.e., 60°) are strongly correlated ( R = 0.95 and 0.95, respectively) with the Ångström exponent. The latter has a meaningful variation with respect to the changes in the complex refractive index of the atmospheric aerosols. Furthermore the polarized phase function shows a moderate negative correlation with respect to the atmospheric aerosol optical depth and single-scattering albedo ( R = −0.76 and −0.33, respectively). Therefore the polarized phase function can be regarded as a key parameter to characterize the atmospheric particles of the region – a populated city in the semi-arid area and surrounded by some dust sources of the Earth's dust belt.

Description: Investigation of ground-based microwave radiometer calibration techniques at 530 hPa Atmospheric Measurement Techniques, 6, 2641-2658, 2013 Author(s): G. Maschwitz, U. Löhnert, S. Crewell, T. Rose, and D. D. Turner Ground-based microwave radiometers (MWR) are becoming more and more common for remotely sensing the atmospheric temperature and humidity profile as well as path-integrated cloud liquid water content. The calibration accuracy of the state-of-the-art MWR HATPRO-G2 (Humidity And Temperature Profiler – Generation 2) was investigated during the second phase of the Radiative Heating in Underexplored Bands Campaign (RHUBC-II) in northern Chile (5320 m above mean sea level, 530 hPa) conducted by the Atmospheric Radiation Measurement (ARM) program conducted between August and October 2009. This study assesses the quality of the two frequently used liquid nitrogen and tipping curve calibrations by performing a detailed error propagation study, which exploits the unique atmospheric conditions of RHUBC-II. Both methods are known to have open issues concerning systematic offsets and calibration repeatability. For the tipping curve calibration an uncertainty of ±0.1 to ±0.2 K (K-band) and ±0.6 to ±0.7 K (V-band) is found. The uncertainty in the tipping curve calibration is mainly due to atmospheric inhomogeneities and the assumed air mass correction for the Earth curvature. For the liquid nitrogen calibration the estimated uncertainty of ±0.3 to ±1.6 K is dominated by the uncertainty of the reflectivity of the liquid nitrogen target. A direct comparison between the two calibration techniques shows that for six of the nine channels that can be calibrated with both methods, they agree within the assessed uncertainties. For the other three channels the unexplained discrepancy is below 0.5 K. Systematic offsets, which may cause the disagreement of both methods within their estimated uncertainties, are discussed.

Description: A new stratospheric and tropospheric NO 2 retrieval algorithm for nadir-viewing satellite instruments: applications to OMI Atmospheric Measurement Techniques, 6, 2607-2626, 2013 Author(s): E. J. Bucsela, N. A. Krotkov, E. A. Celarier, L. N. Lamsal, W. H. Swartz, P. K. Bhartia, K. F. Boersma, J. P. Veefkind, J. F. Gleason, and K. E. Pickering We describe a new algorithm for the retrieval of nitrogen dioxide (NO 2 ) vertical columns from nadir-viewing satellite instruments. This algorithm (SP2) is the basis for the Version 2.1 OMI This algorithm (SP2) is the basis for the Version 2.1 Ozone Monitoring Instrument (OMI) NO 2 Standard Product and features a novel method for separating the stratospheric and tropospheric columns. NO 2 Standard Product and features a novel method for separating the stratospheric and tropospheric columns. The approach estimates the stratospheric NO 2 directly from satellite data without using stratospheric chemical transport models or assuming any global zonal wave pattern. Tropospheric NO 2 columns are retrieved using air mass factors derived from high-resolution radiative transfer calculations and a monthly climatology of NO 2 profile shapes. We also present details of how uncertainties in the retrieved columns are estimated. The sensitivity of the retrieval to assumptions made in the stratosphere–troposphere separation is discussed and shown to be small, in an absolute sense, for most regions. We compare daily and monthly mean global OMI NO 2 retrievals using the SP2 algorithm with those of the original Version 1 Standard Product (SP1) and the Dutch DOMINO product. The SP2 retrievals yield significantly smaller summertime tropospheric columns than SP1, particularly in polluted regions, and are more consistent with validation studies. SP2 retrievals are also relatively free of modeling artifacts and negative tropospheric NO 2 values. In a reanalysis of an INTEX-B validation study, we show that SP2 largely eliminates an ~20% discrepancy that existed between OMI and independent in situ springtime NO 2 SP1 measurements.

Description: Semi-autonomous sounding selection for OCO-2 Atmospheric Measurement Techniques, 6, 2851-2864, 2013 Author(s): L. Mandrake, C. Frankenberg, C. W. O'Dell, G. Osterman, P. Wennberg, and D. Wunch Many modern instruments generate more data than may be fully processed in a timely manner. For some atmospheric sounders, much of the raw data cannot be processed into meaningful observations due to suboptimal viewing conditions, such as the presence of clouds. Conventional solutions are quick, empirical-threshold filters hand-created by domain experts to weed out unlikely or unreasonable observations, coupled with randomized down sampling when the data volume is still too high. In this paper, we describe a method for the construction of a subsampling and ordering solution that maximizes the likelihood that a requested data subset will be usefully processed. The method can be used for any metadata-rich source and implicitly discerns informative vs. non-informative data features while still permitting user feedback into the final features selected for filter implementation. We demonstrate the method by creating a selector for the spectra of the Japanese GOSAT satellite designed to measure column averaged mixing ratios of greenhouse gases including carbon dioxide (CO 2 ). This is done within the Atmospheric CO 2 Measurements from Space (ACOS) NASA project with the intention of eventual use during the early Orbiting Carbon Observatory-2 (OCO-2) mission. OCO-2 will have a 1.5 orders of magnitude larger data volume than ACOS, requiring intelligent pre-filtration.

Description: Global monitoring of terrestrial chlorophyll fluorescence from moderate-spectral-resolution near-infrared satellite measurements: methodology, simulations, and application to GOME-2 Atmospheric Measurement Techniques, 6, 2803-2823, 2013 Author(s): J. Joiner, L. Guanter, R. Lindstrot, M. Voigt, A. P. Vasilkov, E. M. Middleton, K. F. Huemmrich, Y. Yoshida, and C. Frankenberg Globally mapped terrestrial chlorophyll fluorescence retrievals are of high interest because they can provide information on the functional status of vegetation including light-use efficiency and global primary productivity that can be used for global carbon cycle modeling and agricultural applications. Previous satellite retrievals of fluorescence have relied solely upon the filling-in of solar Fraunhofer lines that are not significantly affected by atmospheric absorption. Although these measurements provide near-global coverage on a monthly basis, they suffer from relatively low precision and sparse spatial sampling. Here, we describe a new methodology to retrieve global far-red fluorescence information; we use hyperspectral data with a simplified radiative transfer model to disentangle the spectral signatures of three basic components: atmospheric absorption, surface reflectance, and fluorescence radiance. An empirically based principal component analysis approach is employed, primarily using cloudy data over ocean, to model and solve for the atmospheric absorption. Through detailed simulations, we demonstrate the feasibility of the approach and show that moderate-spectral-resolution measurements with a relatively high signal-to-noise ratio can be used to retrieve far-red fluorescence information with good precision and accuracy. The method is then applied to data from the Global Ozone Monitoring Instrument 2 (GOME-2). The GOME-2 fluorescence retrievals display similar spatial structure as compared with those from a simpler technique applied to the Greenhouse gases Observing SATellite (GOSAT). GOME-2 enables global mapping of far-red fluorescence with higher precision over smaller spatial and temporal scales than is possible with GOSAT. Near-global coverage is provided within a few days. We are able to show clearly for the first time physically plausible variations in fluorescence over the course of a single month at a spatial resolution of 0.5° × 0.5°. We also show some significant differences between fluorescence and coincident normalized difference vegetation indices (NDVI) retrievals.

Description: Accuracy assessment of water vapour measurements from in situ and remote sensing techniques during the DEMEVAP 2011 campaign at OHP Atmospheric Measurement Techniques, 6, 2777-2802, 2013 Author(s): O. Bock, P. Bosser, T. Bourcy, L. David, F. Goutail, C. Hoareau, P. Keckhut, D. Legain, A. Pazmino, J. Pelon, K. Pipis, G. Poujol, A. Sarkissian, C. Thom, G. Tournois, and D. Tzanos The Development of Methodologies for Water Vapour Measurement (DEMEVAP) project aims at assessing and improving humidity sounding techniques and establishing a reference system based on the combination of Raman lidars, ground-based sensors and GPS. Such a system may be used for climate monitoring, radiosonde bias detection and correction, satellite measurement calibration/validation, and mm-level geodetic positioning with Global Navigation Satellite Systems. A field experiment was conducted in September–October 2011 at Observatoire de Haute-Provence (OHP). Two Raman lidars (IGN mobile lidar and OHP NDACC lidar), a stellar spectrometer (SOPHIE), a differential absorption spectrometer (SAOZ), a sun photometer (AERONET), 5 GPS receivers and 4 types of radiosondes (Vaisala RS92, MODEM M2K2-DC and M10, and Meteolabor Snow White) participated in the campaign. A total of 26 balloons with multiple radiosondes were flown during 16 clear nights. This paper presents preliminary findings from the analysis of all these data sets. Several classical Raman lidar calibration methods are evaluated which use either Vaisala RS92 measurements, point capacitive humidity measurements, or GPS integrated water vapour (IWV) measurements. A novel method proposed by Bosser et al. (2010) is also tested. It consists in calibrating the lidar measurements during the GPS data processing. The methods achieve a repeatability of 4–5%. Changes in the calibration factor of IGN Raman lidar are evidenced which are attributed to frequent optical re-alignments. When modelling and correcting the changes as a linear function of time, the precision of the calibration factors improves to 2–3%. However, the variations in the calibration factor, and hence the absolute accuracy, between methods and types of reference data remain at the level of 7%. The intercomparison of radiosonde measurements shows good agreement between RS92 and Snow White measurements up to 12 km. An overall dry bias is found in the measurements from both MODEM radiosondes. Investigation of situations with low RH values ( 〈 10%RH) in the lower and middle troposphere reveals, on occasion, a lower RH detection limit in the Snow White measurements compared to RS92 due to a saturation of the Peltier device. However, on other occasions, a dry bias is found in RS92, instead. On average, both RS92 and Snow White measurements show a slight moist bias at night-time compared to GPS IWV, while the MODEM measurements show a large dry bias. The IWV measurements from SOPHIE (night-time) and SAOZ (daytime) spectrometers, AERONET photometer (daytime) and calibrated Raman lidar (night-time) showed excellent agreement with the GPS IWV measurements.

Description: Evaluating CALIPSO's 532 nm lidar ratio selection algorithm using AERONET sun photometers in Brazil Atmospheric Measurement Techniques, 6, 3281-3299, 2013 Author(s): F. J. S. Lopes, E. Landulfo, and M. A. Vaughan Since the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite first began probing the Earth's atmosphere on 13 June 2006, several research groups dedicated to investigating the atmosphere's optical properties have conducted measurement campaigns to validate the CALIPSO data products. Recently, in order to address the lack of CALIPSO validation studies in the Southern Hemisphere, and especially the South American continent, the Lasers Environmental Applications Research Group at Brazil's Nuclear and Energy Research Institute (IPEN) initiated efforts to assess CALIPSO's aerosol lidar ratio estimates using the AERONET sun photometers installed at five different locations in Brazil. In this study we develop a validation methodology to evaluate the accuracy of the modeled values of the lidar ratios used by the CALIPSO extinction algorithms. We recognize that the quality of any comparisons between satellite and ground-based measurements depends on the degree to which the instruments are collocated, and that even selecting the best spatial and temporal matches does not provide an unequivocal guarantee that both instruments are measuring the same air mass. The validation methodology presented in this study therefore applies backward and forward air mass trajectories in order to obtain the best possible match between the air masses sampled by the satellite and the ground-based instruments, and thus reduces the uncertainties associated with aerosol air mass variations. Quantitative comparisons of lidar ratios determined from the combination of AERONET optical depth measurements and CALIOP integrated attenuated backscatter measurements show good agreement with the model values assigned by the CALIOP algorithm. These comparisons yield a mean percentage difference of −1.5% ± 24%. This result confirms the accuracy in the lidar ratio estimates provided by the CALIOP algorithms over Brazil to within an uncertainty range of no more than 30%.

Description: Characterization of an aerodynamic lens for transmitting particles greater than 1 micrometer in diameter into the Aerodyne aerosol mass spectrometer Atmospheric Measurement Techniques, 6, 3271-3280, 2013 Author(s): L. R. Williams, L. A. Gonzalez, J. Peck, D. Trimborn, J. McInnis, M. R. Farrar, K. D. Moore, J. T. Jayne, W. A. Robinson, D. K. Lewis, T. B. Onasch, M. R. Canagaratna, A. Trimborn, M. T. Timko, G. Magoon, R. Deng, D. Tang, E. de la Rosa Blanco, A. S. H. Prévôt, K. A. Smith, and D. R. Worsnop We have designed and characterized a new inlet and aerodynamic lens for the Aerodyne aerosol mass spectrometer (AMS) that transmits particles between 80 nm and more than 3 μm in vacuum aerodynamic diameter. The design of the inlet and lens was optimized with computational fluid dynamics (CFD) modeling of particle trajectories. Major changes include a redesigned critical orifice holder and valve assembly, addition of a relaxation chamber behind the critical orifice, and a higher lens operating pressure. The transmission efficiency of the new inlet and lens was characterized experimentally with size-selected particles. Experimental measurements are in good agreement with the calculated transmission efficiency.

Description: Multispectral information from TANSO-FTS instrument – Part 2: Application to aerosol effect on greenhouse gas retrievals Atmospheric Measurement Techniques, 6, 3313-3323, 2013 Author(s): H. Herbin, L. C. Labonnote, and P. Dubuisson This article is the second in a series of studies investigating the benefits of multispectral measurements to improve the atmospheric parameter retrievals. In the first paper, we presented an information content (IC) analysis from the thermal infrared (TIR) and shortwave infrared (SWIR) bands of Thermal And Near infrared Sensor for carbon Observations–Fourier Transform Spectrometer (TANSO-FTS) instrument dedicated to greenhouse gas retrieval in clear sky conditions. This second paper presents the potential of the spectral synergy from TIR to visible for aerosol characterization, and their impact on the retrieved CO 2 and CH 4 column concentrations. The IC is then used to determine the most informative spectral channels for the simultaneous retrieval of greenhouse gas total columns and aerosol parameters. The results show that a channel selection spanning the four bands can improve the computation time and retrieval accuracy. Therefore, the spectral synergy allows obtaining up to almost seven different aerosol parameters, which is comparable to the most informative dedicated instruments. Moreover, a channel selection from the TIR to visible bands allows retrieving CO 2 and CH 4 total columns simultaneously in the presence of one aerosol layer with a similar accuracy to using all channels together to retrieve each gas separately in clear sky conditions.

Description: Multispectral information from TANSO-FTS instrument – Part 1: Application to greenhouse gases (CO 2 and CH 4 ) in clear sky conditions Atmospheric Measurement Techniques, 6, 3301-3311, 2013 Author(s): H. Herbin, L. C. Labonnote, and P. Dubuisson The Greenhouse gases Observing SATellite (GOSAT) mission, and in particular the Thermal And Near infrared Sensor for carbon Observations–Fourier Transform Spectrometer (TANSO-FTS) instrument, has the advantage of being able to measure simultaneously the same field of view in different spectral ranges with a high spectral resolution. These features allow studying the benefits of using multispectral measurements to improve the CO 2 and CH 4 retrievals. In order to quantify the impact of the spectral synergy on the retrieval accuracy, we performed an information content (IC) analysis from simulated spectra corresponding to the three infrared bands of TANSO-FTS. The advantages and limitations of using thermal and shortwave infrared simultaneously are discussed according to surface type and state vector composition. The IC is then used to determine the most informative spectral channels for the simultaneous retrieval of CO 2 and CH 4 . The results show that a channel selection spanning the three infrared bands can improve the computation time and retrieval accuracy. Therefore, a selection of less than 700 channels from the thermal infrared (TIR) and shortwave infrared (SWIR) bands allows retrieving CO 2 and CH 4 simultaneously with a similar accuracy to using all channels together to retrieve each gas separately.

Description: Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations Atmospheric Measurement Techniques, 6, 3243-3255, 2013 Author(s): A. Nemuc, J. Vasilescu, C. Talianu, L. Belegante, and D. Nicolae Multi-wavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentration profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δ part ) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δ part of 3%, while for the high depolarizing component (mineral dust) a mean δ part of 35% was assumed. For this study 11 months of lidar measurements were analysed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical in distinguishing between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

Description: Radar-radiometer retrievals of cloud number concentration and dispersion parameter in nondrizzling marine stratocumulus Atmospheric Measurement Techniques, 6, 1817-1828, 2013 Author(s): J. Rémillard, P. Kollias, and W. Szyrmer The retrieval of cloud microphysical properties from remote sensors is challenging. In the past, ground-based radar-radiometer measurements have been successfully used to retrieve the liquid water content profile in nondrizzling clouds but offer little constraint in retrieving other moments of the cloud particle size distribution (PSD). Here, a microphysical condensational model under steady-state supersaturation conditions is utilized to provide additional constraints to the well-established radar-radiometer retrieval techniques. The coupling of the model with the observations allows the retrieval of the three parameters of a lognormal PSD, with two of them being height dependent. Two periods of stratocumulus from the Azores are used to evaluate the novel technique. The results appear reasonable in two nondrizzling periods: continental-like number concentrations are retrieved, in agreement with the drizzle-free cloud conditions. The cloud optical depth derived from the retrieved distributions compares well in magnitude and variability with the one derived independently from a narrow field of view zenith radiometer. Uncertainties coming from the measurements are propagated to the retrieved quantities to estimate their errors. In general, errors smaller than 20% should be attainable for most parameters, demonstrating the added value of the new technique.

Description: Atmospheric CO 2 , δ(O 2 /N 2 ) and δ 13 CO 2 measurements at Jungfraujoch, Switzerland: results from a flask sampling intercomparison program Atmospheric Measurement Techniques, 6, 1805-1815, 2013 Author(s): I. T. van der Laan-Luijkx, S. van der Laan, C. Uglietti, M. F. Schibig, R. E. M. Neubert, H. A. J. Meijer, W. A. Brand, A. Jordan, J. M. Richter, M. Rothe, and M. C. Leuenberger We present results from an intercomparison program of CO 2 , δ(O 2 /N 2 ) and δ 13 CO 2 measurements from atmospheric flask samples. Flask samples are collected on a bi-weekly basis at the High Altitude Research Station Jungfraujoch in Switzerland for three European laboratories: the University of Bern, Switzerland, the University of Groningen, the Netherlands and the Max Planck Institute for Biogeochemistry in Jena, Germany. Almost 4 years of measurements of CO 2 , δ(O 2 /N 2 ) and δ 13 CO 2 are compared in this paper to assess the measurement compatibility of the three laboratories. While the average difference for the CO 2 measurements between the laboratories in Bern and Jena meets the required compatibility goal as defined by the World Meteorological Organization, the standard deviation of the average differences between all laboratories is not within the required goal. However, the obtained annual trend and seasonalities are the same within their estimated uncertainties. For δ(O 2 /N 2 ) significant differences are observed between the three laboratories. The comparison for δ 13 CO 2 yields the least compatible results and the required goals are not met between the three laboratories. Our study shows the importance of regular intercomparison exercises to identify potential biases between laboratories and the need to improve the quality of atmospheric measurements.

Description: High-precision analysis of SF 6 at ambient level Atmospheric Measurement Techniques, 6, 2293-2299, 2013 Author(s): J. S. Lim, D. M. Moon, J. S. Kim, W.-T. Yun, and J. Lee This work reports on the development of a technique for the precise analysis of ambient SF 6 . This technique, which involves a gas chromatograph/electron capture detector (GC-ECD) coupled with an Activated Alumina-F1 (AA-F1) column, performed well in the measurements, particularly in terms of accuracy, which complies with the World Meteorological Organization (WMO)-recommended compatibility of 0.02 ppt. Compared to the Porapak Q technique, we observed a sharper peak shape for the SF 6 stream, which substantiates the improvement in the analytical precision. The traceability to the WMO scale was tested by calibrating the GC-ECD/AA-F1 analyser using five SF 6 standards provided by the WMO/Global Atmosphere Watch (GAW) Central Calibration Laboratory (CCL) for SF 6 (NOAA, United States of America). After calibration by various methods, the GC-ECD/AA-F1 accurately estimated the mole fraction of SF 6 in the working standard prepared by the World Calibration Centre for SF 6 operated by the Korea Meteorological Administration (KMA)/Korea Research Institute of Standards and Science (KRISS). Among the calibration methods, the two-point calibration method emerged to be the most economical procedure in terms of the data quality and measurement time. It was found that the KRISS scale of SF 6 /N 2 was biased by 0.13 ppt when compared to the WMO scale of SF 6 /air; this bias is probably due to a different matrix.

Description: Aircraft based four-channel thermal dissociation laser induced fluorescence instrument for simultaneous measurements of NO 2 , total peroxy nitrate, total alkyl nitrate, and HNO 3 Atmospheric Measurement Techniques, 6, 971-980, 2013 Author(s): P. Di Carlo, E. Aruffo, M. Busilacchio, F. Giammaria, C. Dari-Salisburgo, F. Biancofiore, G. Visconti, J. Lee, S. Moller, C. E. Reeves, S. Bauguitte, G. Forster, R. L. Jones, and B. Ouyang A four-channel thermal dissociation laser induced fluorescence (TD-LIF) instrument has been developed for simultaneous measurements of nitrogen dioxide (NO 2 ), total peroxy nitrate (∑PNs), total alkyl nitrate (∑ANs) and nitric acid (HNO 3 ). NO 2 is measured directly by LIF at 532 nm, whereas organic nitrates and nitric acid are thermally dissociated at distinct temperatures in the inlet to form NO 2 , which is then measured by LIF. The concentrations of each dissociated species are derived by the differences in measured NO 2 relative to the reference colder inlet channel. The TD-LIF was adapted to fly on board the UK Facility for Airborne Atmospheric Measurements (FAAM) BAe 146-301 atmospheric research aircraft in summer 2010, and to date has successfully flown in five field campaigns. This paper reports novel improvements in the TD-LIF instrumentations, including (1) the use of a single wavelength laser, which makes the system compact and relatively cheap; (2) the use of a single beam laser that allows easy alignment and optical stability against the vibrational aircraft environment; and (3) the optical assembly of four detection cells that allow simultaneous and fast (time resolution up to 0.1 s) measurements of NO 2 , ∑PNs, ∑ANs and HNO 3 . Laboratory-generated mixtures of PNs, ANs and HNO 3 in zero air are converted into NO 2 and used to fix the dissociation temperatures of each heated inlet to test the selectivity of the instrument and potential interferences due to recombination reactions of the dissociated products. The effectiveness of the TD-LIF was demonstrated during the RONOCO aircraft campaign (summer 2010). A chemiluminescence system that was measuring NO 2 and a broadband cavity enhanced absorption spectrometer (BBCEAS) that was measuring one of the PNs (N 2 O 5 ) were installed on the same aircraft during the campaign. The in-flight intercomparison of the new TD-LIF with the chemiluminescence system for NO 2 measurements and the intercomparison between ∑PNs measured by the TD-LIF and N 2 O 5 by the BBCEAS are used to assess the performance of the TD-LIF.

Description: Maintaining consistent traceability in high-precision isotope measurements of CO 2 : a way to verify atmospheric trends of δ 13 C and δ 18 O Atmospheric Measurement Techniques, 6, 1685-1705, 2013 Author(s): L. Huang, A. Chivulescu, D. Ernst, W. Zhang, A.-L. Norman, and Y.-S. Lee Maintaining consistent traceability of high-precision measurements of CO 2 isotopes is critical in order to obtain accurate atmospheric trends of δ 13 C and δ 18 O (in CO 2 ). Although a number of laboratories/organizations around the world have been conducting baseline measurements of atmospheric CO 2 isotopes for several decades, reports on the traceability and maintenance are rare. In this paper, a principle and an approach for maintaining consistent traceability in high-precision isotope measurements (δ 13 C and δ 18 O) of atmospheric CO 2 are described. The concept of Big Delta is introduced and its role in maintaining traceability of the isotope measurements is described and discussed extensively. The uncertainties of the traceability have been estimated based on annual calibration records over the last 10 yr. The overall uncertainties of CO 2 isotope measurements for individual ambient samples analyzed by the program at Environment Canada have been estimated (excluding these associated with the sampling). The values are 0.02 and 0.05‰ in δ 13 C and δ 18 O, respectively, which are close to the World Meteorological Organization (WMO) targets for data compatibility. The annual rates of change in δ 13 C and δ 18 O of the primary anchor (which links the flask measurements back to the VPDB-CO 2 scale) are close to zero (−0.0016 ± 0.0012‰, and −0.006 ± 0.003‰ per year, respectively) over a period of 10 yr (2001–2011). The average annual changes of δ 13 C and δ 18 O in air CO 2 at Alert GAW station over the period from 1999 to 2010 have been evaluated and confirmed; they are −0.025 ± 0.003‰ and 0.000 ± 0.010‰, respectively. The results are consistent with a continuous contribution of fossil fuel CO 2 to the atmosphere, having a trend toward more negative in δ 13 C, whereas the lack of change in δ 18 O likely reflects the influence from the global hydrologic cycle. The total change of δ 13 C and δ 18 O during this period is ~0.27‰ and ~0.00‰, respectively. Finally, the challenges and recommendations as strategies to maintain a consistent traceability are described.

Description: Measurements of air pollution emission factors for marine transportation in SECA Atmospheric Measurement Techniques, 6, 1777-1791, 2013 Author(s): B. Alföldy, J. B. Lööv, F. Lagler, J. Mellqvist, N. Berg, J. Beecken, H. Weststrate, J. Duyzer, L. Bencs, B. Horemans, F. Cavalli, J.-P. Putaud, G. Janssens-Maenhout, A. P. Csordás, R. Van Grieken, A. Borowiak, and J. Hjorth The chemical composition of the plumes of seagoing ships was measured during a two week long measurement campaign in the port of Rotterdam, Hoek van Holland The Netherlands, in September 2009. Altogether, 497 ships were monitored and a statistical evaluation of emission factors (g kg −1 fuel) was provided. The concerned main atmospheric components were SO 2 , NO 2 , NO x and the aerosol particle number. In addition, the elemental and water-soluble ionic composition of the emitted particulate matter was determined. Emission factors were expressed as a function of ship type, power and crankshaft rotational speed. The average SO 2 emission factor was found to be roughly half of what is allowed in sulphur emission control areas (16 vs. 30 g kg −1 fuel), and exceedances of this limit were rarely registered. A significant linear relationship was observed between the SO 2 and particle number emission factors. The intercept of the regression line, 4.8 × 10 15 (kg fuel) −1 , gives the average number of particles formed during the burning of 1 kg zero sulphur content fuel, while the slope, 2 × 10 18 , provides the average number of particles formed with 1 kg sulphur burnt with the fuel. Water-soluble ionic composition analysis of the aerosol samples from the plumes showed that ~144 g of particulate sulphate was emitted from 1 kg sulphur burnt with the fuel. The mass median diameter of sulphate particles estimated from the measurements was ~42 nm.

Description: Evaluation of the Lidar/Radiometer Inversion Code (LIRIC) to determine microphysical properties of volcanic and desert dust Atmospheric Measurement Techniques, 6, 1707-1724, 2013 Author(s): J. Wagner, A. Ansmann, U. Wandinger, P. Seifert, A. Schwarz, M. Tesche, A. Chaikovsky, and O. Dubovik The Lidar/Radiometer Inversion Code (LIRIC) combines the multiwavelength lidar technique with sun/sky photometry and allows us to retrieve vertical profiles of particle optical and microphysical properties separately for fine-mode and coarse-mode particles. After a brief presentation of the theoretical background, we evaluate the potential of LIRIC to retrieve the optical and microphysical properties of irregularly shaped dust particles. The method is applied to two very different aerosol scenarios: a strong Saharan dust outbreak towards central Europe and an Eyjafjallajökull volcanic dust event. LIRIC profiles of particle mass concentrations for the coarse-mode as well as for the non-spherical particle fraction are compared with results for the non-spherical particle fraction as obtained with the polarization-lidar-based POLIPHON method. Similar comparisons for fine-mode and spherical particle fractions are presented also. Acceptable agreement between the different dust mass concentration profiles is obtained. LIRIC profiles of optical properties such as particle backscatter coefficient, lidar ratio, Ångström exponent, and particle depolarization ratio are compared with direct Raman lidar observations. Systematic deviations between the LIRIC retrieval products and the Raman lidar measurements of the desert dust lidar ratio, depolarization ratio, and spectral dependencies of particle backscatter and lidar ratio point to the applied spheroidal-particle model as main source for these uncertainties in the LIRIC results.

Description: MODIS 3 km aerosol product: applications over land in an urban/suburban region Atmospheric Measurement Techniques, 6, 1747-1759, 2013 Author(s): L. A. Munchak, R. C. Levy, S. Mattoo, L. A. Remer, B. N. Holben, J. S. Schafer, C. A. Hostetler, and R. A. Ferrare MODerate resolution Imaging Spectroradiometer (MODIS) instruments aboard the Terra and Aqua satellites have provided a rich dataset of aerosol information at a 10 km spatial scale. Although originally intended for climate applications, the air quality community quickly became interested in using the MODIS aerosol data. However, 10 km resolution is not sufficient to resolve local scale aerosol features. With this in mind, MODIS Collection 6 includes a global aerosol product with a 3 km resolution. Here, we evaluate the 3 km product over the Baltimore–Washington D.C., USA, corridor during the summer of 2011 by comparing with spatially dense aerosol data measured by airborne High Spectral Resolution Lidar (HSRL) and a network of 44 sun photometers (SP) spaced approximately 10 km apart, collected as part of the DISCOVER-AQ field campaign. The HSRL instrument shows that AOD can vary by over 0.2 within a single 10 km MODIS pixel, meaning that higher resolution satellite retrievals may help to better characterize aerosol spatial distributions in this region. Different techniques for validating a high-resolution aerosol product against SP measurements are considered. Although the 10 km product is more statistically reliable than the 3 km product, the 3 km product still performs acceptably with nearly two-thirds of MODIS/SP collocations falling within an expected error envelope with high correlation ( R 〉 0.90), although with a high bias of ~ 0.06. The 3 km product can better resolve aerosol gradients and retrieve closer to clouds and shorelines than the 10 km product, but tends to show more noise, especially in urban areas. This urban degradation is quantified using ancillary land cover data. Overall, we show that the MODIS 3 km product adds new information to the existing set of satellite derived aerosol products and validates well over the region, but due to noise and problems in urban areas, should be treated with some degree of caution.

Description: Calibration and validation of the advanced E-Region Wind Interferometer Atmospheric Measurement Techniques, 6, 1761-1776, 2013 Author(s): S. K. Kristoffersen, W. E. Ward, S. Brown, and J. R. Drummond The advanced E-Region Wind Interferometer (ERWIN II) combines the imaging capabilities of a CCD detector with the wide field associated with field-widened Michelson interferometry. This instrument is capable of simultaneous multi-directional wind observations for three different airglow emissions (oxygen green line (O( 1 S)) at a height of ~97 km, the P Q(7) and P (7) emission lines in the O 2 (0–1) atmospheric band at ~93 km and P 1 (3) emission line in the (6, 2) hydroxyl Meinel band at ~87 km) on a three minute cadence. In each direction, for 45 s measurements for typical airglow volume emission rates, the instrument is capable of line-of-sight wind precisions of ~1 m s −1 for hydroxyl and O( 1 S) and ~4 m s −1 for O 2 . This precision is achieved using a new data analysis algorithm which takes advantage of the imaging capabilities of the CCD detector along with knowledge of the instrument phase variation as a function of pixel location across the detector. This instrument is currently located in Eureka, Nunavut as part of the Polar Environment Atmospheric Research Laboratory (PEARL) (80°N, 86° W). The details of the physical configuration, the data analysis algorithm, the measurement calibration and validation of the observations from December 2008 and January 2009 are described. Field measurements which demonstrate the capabilities of this instrument are presented. To our knowledge, the wind determinations with this instrument are the most accurate and have the highest observational cadence for airglow wind observations of this region of the atmosphere and match the capabilities of other wind-measuring techniques.

Description: Validation of middle-atmospheric campaign-based water vapour measured by the ground-based microwave radiometer MIAWARA-C Atmospheric Measurement Techniques, 6, 1725-1745, 2013 Author(s): B. Tschanz, C. Straub, D. Scheiben, K. A. Walker, G. P. Stiller, and N. Kämpfer Middle atmospheric water vapour can be used as a tracer for dynamical processes. It is mainly measured by satellite instruments and ground-based microwave radiometers. Ground-based instruments capable of measuring middle-atmospheric water vapour are sparse but valuable as they complement satellite measurements, are relatively easy to maintain and have a long lifetime. MIAWARA-C is a ground-based microwave radiometer for middle-atmospheric water vapour designed for use on measurement campaigns for both atmospheric case studies and instrument intercomparisons. MIAWARA-C's retrieval version 1.1 (v1.1) is set up in a such way as to provide a consistent data set even if the instrument is operated from different locations on a campaign basis. The sensitive altitude range for v1.1 extends from 4 hPa (37 km) to 0.017 hPa (75 km). For v1.1 the estimated systematic error is approximately 10% for all altitudes. At lower altitudes it is dominated by uncertainties in the calibration, with altitude the influence of spectroscopic and temperature uncertainties increases. The estimated random error increases with altitude from 5 to 25%. MIAWARA-C measures two polarisations of the incident radiation in separate receiver channels, and can therefore provide two measurements of the same air mass with independent instrumental noise. The standard deviation of the difference between the profiles obtained from the two polarisations is in excellent agreement with the estimated random measurement error of v1.1. In this paper, the quality of v1.1 data is assessed for measurements obtained at two different locations: (1) a total of 25 months of measurements in the Arctic (Sodankylä, 67.37° N, 26.63° E) and (2) nine months of measurements at mid-latitudes (Zimmerwald, 46.88° N, 7.46° E). For both locations MIAWARA-C's profiles are compared to measurements from the satellite experiments Aura MLS and MIPAS. In addition, comparisons to ACE-FTS and SOFIE are presented for the Arctic and to the ground-based radiometer MIAWARA for the mid-latitude campaigns. In general, all intercomparisons show high correlation coefficients, confirming the ability of MIAWARA-C to monitor temporal variations of the order of days. The biases are generally below 13% and within the estimated systematic uncertainty of MIAWARA-C. No consistent wet or dry bias is identified for MIAWARA-C. In addition, comparisons to the reference instruments indicate the estimated random error of v1.1 to be a realistic measure of the random variation on the retrieved profile between 45 and 70 km.

Description: A comparison of rainfall measurements from multiple instruments Atmospheric Measurement Techniques, 6, 1585-1595, 2013 Author(s): X. C. Liu, T. C. Gao, and L. Liu Simultaneous observations of rainfall collected by a tipping bucket rain gauge (TBRG), a weighing rain gauge (WRG), an optical rain gauge (ORG), a present weather detector (PWD), a Joss–Waldvogel disdrometer (JWD), and a 2-D video disdrometer (2DVD) during January to October 2012 were analyzed to evaluate how accurately they measure rainfall and drop size distributions (DSDs). For the long-term observations, there were different discrepancies in rain amounts from six instruments on the order of 0% to 27.7%. The TBRG, WRG, and ORG have a good agreement, while the PWD and 2DVD record higher and the JWD lower rain rates when R 〉 20 mm h −1 , the ORG agrees well with JWD and 2DVD, while the TBRG records higher and the WRG lower rain rates when R 〉 20 mm h −1 . Compared with the TBRG and WRG, optical and impact instruments can measure the rain rate accurately in the light rain. The overall DSDs of JWD and 2DVD agree well with each other, except for the small raindrops ( D 〈 1 mm). JWD can measure more moderate-size raindrops (0.3 mm 〈 D 〈 1.5 mm) than 2DVD, but 2DVD can measure more small-size raindrops ( D 〈 0.3 mm). 2DVD has a larger measurement range; more overall raindrops can be measured by 2DVD than by JWD in different rain rate regimes. But small raindrops might be underestimated by 2DVD when R 〉 15 mm h −1 . The small raindrops tend to be omitted in the more large-size raindrops due to the shadow effect of light. Therefore, the measurement accuracy of small raindrops in the heavy rainfall from 2DVD should be handled carefully.

Description: Time series inversion of spectra from ground-based radiometers Atmospheric Measurement Techniques, 6, 1597-1609, 2013 Author(s): O. M. Christensen and P. Eriksson Retrieving time series of atmospheric constituents from ground-based spectrometers often requires different temporal averaging depending on the altitude region in focus. This can lead to several datasets existing for one instrument, which complicates validation and comparisons between instruments. This paper puts forth a possible solution by incorporating the temporal domain into the maximum a posteriori (MAP) retrieval algorithm. The state vector is increased to include measurements spanning a time period, and the temporal correlations between the true atmospheric states are explicitly specified in the a priori uncertainty matrix. This allows the MAP method to effectively select the best temporal smoothing for each altitude, removing the need for several datasets to cover different altitudes. The method is compared to traditional averaging of spectra using a simulated retrieval of water vapour in the mesosphere. The simulations show that the method offers a significant advantage compared to the traditional method, extending the sensitivity an additional 10 km upwards without reducing the temporal resolution at lower altitudes. The method is also tested on the Onsala Space Observatory (OSO) water vapour microwave radiometer confirming the advantages found in the simulation. Additionally, it is shown how the method can interpolate data in time and provide diagnostic values to evaluate the interpolated data.

Description: Development and testing of an online method to measure ambient fine particulate reactive oxygen species (ROS) based on the 2',7'-dichlorofluorescin (DCFH) assay Atmospheric Measurement Techniques, 6, 1647-1658, 2013 Author(s): L. E. King and R. J. Weber An online, semi-continuous instrument to measure fine particle (PM 2.5 ) reactive oxygen species (ROS) was developed based on the fluorescent probe 2'7'-dichlorofluorescin (DCFH). Parameters that influence probe response were first characterized to develop an optimal method for use in a field instrument. The online method used a mist chamber scrubber to collect total (gas plus particle) ROS components (ROS t ) alternating with gas phase ROS (ROS g ) by means of an inline filter. Particle phase ROS (ROS p ) was determined by the difference between ROS t and ROS g . The instrument was deployed in urban Atlanta, Georgia, USA, and at a rural site during various seasons. Concentrations from the online instrument generally agreed well with those from an intensive filter measurement of ROS p . Concentrations of the ROS p measurements made with this instrument were lower than reported in other studies, often below the instrument's average limit of detection (0.15 nmol H 2 O 2 equivalents m −3 ). Mean ROS p concentrations were 0.26 nmol H 2 O 2 equivalents m −3 at the Atlanta urban sites compared to 0.14 nmol H 2 O 2 equivalents m −3 at the rural site.

Description: Towards a stable and absolute atmospheric carbon dioxide instrument using spectroscopic null method Atmospheric Measurement Techniques, 6, 1611-1621, 2013 Author(s): B. Xiang, D. D. Nelson, J. B. McManus, M. S. Zahniser, and S. C. Wofsy We present a novel spectral method to measure atmospheric carbon dioxide (CO 2 ) with high precision and stability without resorting to calibration tanks during long-term operation. This spectral null method improves precision by reducing spectral proportional noise associated with laser emission instabilities. We employ sealed quartz cells with known CO 2 column densities to serve as the permanent internal references in the null method, which improve the instrument's stability and accuracy. A prototype instrument – AB solute C arbon dioxide (ABC) is developed using this new approach. The instrument has a one-second precision of 0.02 ppm, which averages down to 0.007 ppm within one minute. Long-term stability of within 0.1 ppm is achieved without any calibrations for over a one-month period. These results have the potential for eliminating the need for calibration cylinders for high accuracy field measurements of carbon dioxide.

Description: Averaging kernel prediction from atmospheric and surface state parameters based on multiple regression for nadir-viewing satellite measurements of carbon monoxide and ozone Atmospheric Measurement Techniques, 6, 1633-1646, 2013 Author(s): H. M. Worden, D. P. Edwards, M. N. Deeter, D. Fu, S. S. Kulawik, J. R. Worden, and A. Arellano A current obstacle to the observation system simulation experiments (OSSEs) used to quantify the potential performance of future atmospheric composition remote sensing systems is a computationally efficient method to define the scene-dependent vertical sensitivity of measurements as expressed by the retrieval averaging kernels (AKs). We present a method for the efficient prediction of AKs for multispectral retrievals of carbon monoxide (CO) and ozone (O 3 ) based on actual retrievals from MOPITT (Measurements Of Pollution In The Troposphere) on the Earth Observing System (EOS)-Terra satellite and TES (Tropospheric Emission Spectrometer) and OMI (Ozone Monitoring Instrument) on EOS-Aura, respectively. This employs a multiple regression approach for deriving scene-dependent AKs using predictors based on state parameters such as the thermal contrast between the surface and lower atmospheric layers, trace gas volume mixing ratios (VMRs), solar zenith angle, water vapor amount, etc. We first compute the singular value decomposition (SVD) for individual cloud-free AKs and retain the first three ranked singular vectors in order to fit the most significant orthogonal components of the AK in the subsequent multiple regression on a training set of retrieval cases. The resulting fit coefficients are applied to the predictors from a different test set of test retrievals cased to reconstruct predicted AKs, which can then be evaluated against the true retrieval AKs from the test set. By comparing the VMR profile adjustment resulting from the use of the predicted vs. true AKs, we quantify the CO and O 3 VMR profile errors associated with the use of the predicted AKs compared to the true AKs that might be obtained from a computationally expensive full retrieval calculation as part of an OSSE. Similarly, we estimate the errors in CO and O 3 VMRs from using a single regional average AK to represent all retrievals, which has been a common approximation in chemical OSSEs performed to date. For both CO and O 3 in the lower troposphere, we find a significant reduction in error when using the predicted AKs as compared to a single average AK. This study examined data from the continental United States (CONUS) for 2006, but the approach could be applied to other regions and times.

Description: Retrieving wind statistics from average spectrum of continuous-wave lidar Atmospheric Measurement Techniques, 6, 1673-1683, 2013 Author(s): E. Branlard, A. T. Pedersen, J. Mann, N. Angelou, A. Fischer, T. Mikkelsen, M. Harris, C. Slinger, and B. F. Montes The aim of this study is to experimentally demonstrate that the time-average Doppler spectrum of a continuous-wave (cw) lidar is proportional to the probability density function of the line-of-sight velocities. This would open the possibility of using cw lidars for the determination of the second-order atmospheric turbulence statistics. An atmospheric field campaign and a wind tunnel experiment are carried out to show that the use of an average Doppler spectrum instead of a time series of velocities determined from individual Doppler spectra significantly reduces the differences with the standard deviation measured using ordinary anemometers, such as ultra-sonic anemometers or hotwires. The proposed method essentially removes the spatial averaging effect intrinsic to the cw lidar systems.