ALBERT

Description: Quantification of model uncertainty in aerosol optical thickness retrieval from Ozone Monitoring Instrument (OMI) measurements Atmospheric Measurement Techniques Discussions, 6, 8509-8541, 2013 Author(s): A. Määttä, M. Laine, J. Tamminen, and J. P. Veefkind We study uncertainty quantification in remote sensing of aerosols in the atmosphere with top of the atmosphere reflectance measurements from the nadir-viewing Ozone Monitoring Instrument (OMI). Focus is on the uncertainty in aerosol model selection of pre-calculated aerosol models and on the statistical modelling of the model inadequacies. The aim is to apply statistical methodologies that improve the uncertainty estimates of the aerosol optical thickness (AOT) retrieval by propagating model selection and model error related uncertainties more realistically. We utilise Bayesian model selection and model averaging methods for the model selection problem and use Gaussian processes to model the smooth systematic discrepancies from the modelled to observed reflectance. The systematic model error is learned from an ensemble of operational retrievals. The operational OMI multi-wavelength aerosol retrieval algorithm OMAERO is used for cloud free, over land pixels of the OMI instrument with the additional Bayesian model selection and model discrepancy techniques. The method is demonstrated with four examples with different aerosol properties: weakly absorbing aerosols, forest fires over Greece and Russia, and Sahara dessert dust. The presented statistical methodology is general; it is not restricted to this particular satellite retrieval application.

Description: The Greenhouse Gas Climate Change Initiative (GHG-CCI): comparative validation of GHG-CCI SCIAMACHY/ENVISAT and TANSO-FTS/GOSAT CO 2 and CH 4 retrieval algorithm products with measurements from the TCCON network Atmospheric Measurement Techniques Discussions, 6, 8679-8741, 2013 Author(s): B. Dils, M. Buchwitz, M. Reuter, O. Schneising, H. Boesch, R. Parker, S. Guerlet, I. Aben, T. Blumenstock, J. P. Burrows, A. Butz, N. M. Deutscher, C. Frankenberg, F. Hase, O. P. Hasekamp, J. Heymann, M. De Mazière, J. Notholt, R. Sussmann, T. Warneke, D. Griffith, V. Sherlock, and D. Wunch Column-averaged dry-air mole fractions of carbon dioxide and methane have been retrieved from spectra acquired by the TANSO-FTS and SCIAMACHY instruments on board GOSAT and ENVISAT using a range of European retrieval algorithms. These retrievals have been compared with data from ground-based high-resolution Fourier Transform Spectrometers (FTS) from the Total Carbon Column Observing Network (TCCON). The participating algorithms are the Weighting Function Modified Differential Optical Absorption Spectroscopy (DOAS) algorithm (WFMD, University of Bremen), the Bremen Optimal Estimation DOAS algorithm (BESD, University of Bremen), the Iterative Maximum A Posteriori DOAS (IMAP, Jet Propulsion Laboratory (JPL) and Netherlands Institute for Space Research algorithm (SRON)), the proxy and full-physics versions of SRON's RemoTeC algorithm (SRPR and SRFP respectively) and the proxy and full-physics versions of the University of Leicester's adaptation of the OCO (Orbiting Carbon Observatory) algorithm (OCPR and OCFP respectively). The goal of this algorithm inter-comparison was to identify strengths and weaknesses of the various so-called Round Robin data sets generated with the various algorithms so as to determine which of the competing algorithms would proceed to the next round of the European Space Agency's (ESA) Greenhouse Gas Climate Change Initiative (GHG-CCI) project, which is the generation of the so-called Climate Research Data Package (CRDP), which is the first version of the Essential Climate Variable (ECV) "Greenhouse Gases" (GHG). For CO 2 , all algorithms reach the precision requirements for inverse modelling ( 〈 8 ppb), with only WFMD having a lower precision (4.7 ppm) than the other algorithm products (2.4–2.5 ppm). When looking at the seasonal relative accuracy (SRA, variability of the bias in space and time), none of the algorithms have reached the demanding 〈 0.5 ppm threshold. For CH 4 , the precision for both SCIAMACHY products (50.2 ppb for IMAP and 76.4 ppb for WFMD) fail to meet the 〈 34 ppb threshold, but note that this work focusses on the period after the 2005 SCIAMACHY detector degradation. The GOSAT X CH 4 precision ranges between 18.1 and 14.0 ppb. Looking at the SRA, all GOSAT algorithm products reach the 〈 10 ppm threshold (values ranging between 5.4 and 6.2 ppb). For SCIAMACHY, IMAP and WFMD have a SRA of 17.2 ppb and 10.5 ppb respectively.

Description: The effect of phase partitioning of semivolatile compounds on the measured CCN activity of aerosol particles Atmospheric Measurement Techniques Discussions, 6, 8413-8433, 2013 Author(s): S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen The effect of inorganic semivolatile aerosol compounds on the CCN activity of aerosol particles was studied by using a computational model for a DMT-CCN counter, a cloud parcel model for condensation kinetics and experiments to quantify the modelled results. Concentrations of water vapour and semivolatiles as well as aerosol trajectories in the CCN column were calculated by a computational fluid dynamics model. These trajectories and vapour concentrations were then used as an input for the cloud parcel model to simulate mass transfer kinetics of water and semivolatiles between aerosol particles and the gas phase. Two different questions were studied: (1) how big fraction of semivolatiles is evaporated from particles before activation in the CCN counter? (2) How much the CCN activity can be increased due to condensation of semivolatiles prior to the maximum water supersaturation in the case of high semivolatile concentration in the gas phase? The results show that, to increase the CCN activity of aerosol particles, a very high gas phase concentration (as compared to typical ambient conditions) is needed. We used nitric acid as a test compound. A concentration of several ppb or higher is needed for measurable effect. In the case of particle evaporation, we used ammonium nitrate as a test compound and found that it partially evaporates before maximum supersaturation is reached in the CCN counter, thus causing an underestimation of CCN activity. The effect of evaporation is clearly visible in all supersaturations, leading to an underestimation of the critical dry diameter by 10 to 15 nanometres in the case of ammonium nitrate particles in different supersaturations. This result was also confirmed by measurements in supersaturations between 0.1 and 0.7%.

Description: Spectral Aerosol Extinction Monitoring System (SÆMS): setup, observational products, and comparisons Atmospheric Measurement Techniques Discussions, 6, 8647-8677, 2013 Author(s): A. Skupin, A. Ansmann, R. Engelmann, and H. Baars A Spectral Aerosol Extinction Monitoring System (SÆMS) is presented that allows us to continuously measure the spectral extinction coefficient of atmospheric aerosol particles along an about 2.7 km long optical path at 30–50 m height above ground at Leipzig (51.3° N, 12.4° E), Germany. The fully automated instrument measures the ambient aerosol extinction coefficients from 300–1000 nm. The main goal of SÆMS observations are long-term studies of the relationship between particle extinction and relative humidity from below 40 % to almost 100 %. The setup is presented and observations (a case study and statistical results for 2009) are discussed in terms of time series of 550 nm particle optical depth, Ångström exponent, and particle size distribution retrieved from the spectrally resolved extinction. The SÆMS measurements are compared with simultaneously performed EARLINET lidar, AERONET photometer, and in situ aerosol observations of particle size distribution and related extinction coefficients at the roof of our institute. Consistency between the different measurements is found which corroborates the quality of the SÆMS observations.

Description: Validation of SCIAMACHY O 2 A band cloud heights using Cloudnet radar/lidar measurements Atmospheric Measurement Techniques Discussions, 6, 8603-8645, 2013 Author(s): P. Wang and P. Stammes For the first time two SCIAMACHY O 2 A band cloud height products are validated using ground-based radar/lidar measurements between January 2003 and December 2011. The products are the ESA Level 2 (L2) version 5.02 cloud top height and the FRESCO (Fast Retrieval Scheme for Clouds from the Oxygen A band) version 6 cloud height. The radar/lidar profiles are obtained at the Cloudnet sites of Cabauw and Lindenberg, and are averaged for one hour centered at the SCIAMACHY overpass time to achieve an optimal temporal and spatial match. In total we have about 220 cases of single layer clouds and 200 cases of multi-layer clouds. The FRESCO cloud height and ESA L2 cloud top height are compared with the Cloudnet cloud top height and Cloudnet cloud middle height. We find that the ESA L2 cloud top height has a better agreement with the Cloudnet cloud top height than the Cloudnet cloud middle height. The ESA L2 cloud top height is on average 0.44 km higher than the Cloudnet cloud top height, with a standard deviation of 3.07 km. The FRESCO cloud height is closer to the Cloudnet cloud middle height than the Cloudnet cloud top height. The mean difference between the FRESCO cloud height and the Cloudnet cloud middle height is −0.14 km with a standard deviation of 1.88 km. The SCIAMACHY cloud height products are further compared to the Cloudnet cloud top height and the Cloudnet cloud middle height in 1 km bins. For single layer clouds, the difference between the ESA L2 cloud top height and the Cloudnet cloud top height is less than 1 km for each cloud bin at 3–7 km, which is 24 % percent of the data. The difference between the FRESCO cloud height and the Cloudnet cloud middle height is less than 1 km for each cloud bin at 0–6 km, which is 85 % percent of the data. The results are similar for multi-layer clouds, but the percentage of cases having a bias within 1 km is smaller than for single layer clouds. Since globally about 60 % of all clouds are low clouds and 42 % are single-layer low clouds, we expect that globally for a large percentage of cases the FRESCO cloud height would be close to the cloud middle height.

Description: Characteristics of cloud liquid water path from SEVIRI on the Meteosat Second Generation 2 satellite for several cloud types Atmospheric Measurement Techniques Discussions, 6, 8743-8782, 2013 Author(s): A. Kniffka, M. Stengel, M. Lockhoff, R. Bennartz, and R. Hollmann In this study the temporal and spatial characteristics of liquid water path (LWP) of low, middle level and high clouds are analysed using space-based observations of the Spinning Enhanced Visible and Infrared Imager (SEVIRI) onboard the Meteosat Second Generation 2 (MSG2) satellite. Both geophysical quantities are part of the dataset CLAAS (CLoud property dAtAset using SEVIRI) and are generated by EUMETSAT's Satellite Application Facility on Climate Monitoring (CM SAF). In this article we focus on the statistical properties of LWP retrieved at daylight associated with the individual cloud type. Our results reveal that each cloud type possesses a characteristic LWP distribution. These frequency distributions are constant with time in the entire SEVIRI field of view, but vary for smaller regions like Central Europe. The average LWP is higher over land than over sea, in case of low clouds 15–27% for 2009 and the variance of the frequency distributions is enhanced. Also, the average diurnal cycle of LWP is related to cloud type where most pronounced diurnal variations were detected for middle level clouds. With SEVIRI it is possible to distinguish between intrinsic LWP variability and variations driven by cloud amount. The relative amplitude of the intrinsic diurnal cycle can exceed the cloud amount driven amplitude.

Description: Remote sensing of atmospheric trace gas columns: an efficient approach for regularization and calculation of total column averaging kernels Atmospheric Measurement Techniques Discussions, 6, 4999-5031, 2013 Author(s): T. Borsdorff, O. P. Hasekamp, A. Wassmann, and J. Landgraf A concept is proposed to retrieve the vertical column densities of atmospheric trace gases from remote sensing measurements. It combines the numerical simplicity of a least-squares profile scaling retrieval with the numerically robust calculation of the total column averaging kernel using an analytic expression. The approach enables calculation of the total column averaging kernel on arbitrary vertical grids. Formally, the proposed method is equivalent to Tikhonov regularization of the first kind with an infinite regularization strength. Due to its efficiency it is particularly suited for implementation in operational data processing with high demands on processing time. To demonstrate the method, we apply it to CO column retrieval from simulated measurements in the 2.3 μm spectral region and to O 3 column retrieval from the UV, which represents ideal measurements of a series of space-borne spectrometers like SCIAMACHY, TROPOMI, GOME, and GOME-2. For both spectral ranges, we consider clear-sky and cloudy scenes where clouds are modelled as an elevated Lambertian surface. Here, the smoothing error for the clear-sky and cloudy atmosphere is significant and reaches several percent, depending on the reference profile which is used for scaling. This underlines the importance of the column averaging kernel for a proper interpretation of retrieved column densities. Furthermore, we show that the total column smoothing error is affected by a discretization error when total column averaging kernels are not represented on a fine enough vertical grid. For both retrievals this effect becomes negligible by using a vertical grid with 20–40 equally thick layers between 0 and 50 km.

Description: Mixing layer height retrievals by multichannel microwave radiometer observations Atmospheric Measurement Techniques Discussions, 6, 4971-4998, 2013 Author(s): D. Cimini, F. De Angelis, J.-C. Dupont, S. Pal, and M. Haeffelin The mixing layer height (MLH) is a key parameter for boundary layer studies, including meteorology, air quality, and climate. MLH estimates are inferred from in situ radiosonde measurements or remote sensing observations from instruments like lidar, wind profiling radar, or sodar. Methods used to estimate MLH from radiosonde profiles are also used with atmospheric temperature and humidity profiles retrieved by microwave radiometers (MWR). This paper proposes an alternative approach to estimate MLH from MWR data, based on direct observations (brightness temperatures, Tb) instead of retrieved profiles. To our knowledge, MLH estimates directly from Tb observations has never been attempted before. The method consists of a multivariate linear regression trained with an a priori set of collocated MWR Tb observations (multi-frequency and multi-angle) and MLH estimates from a state-of-the-art lidar system. Results show that the method is able to follow both the diurnal cycle and the day-to-day variability as suggested by the lidar measurements, and also it can detect low MLH values that are below the full overlap limit (~ 200 m) of the lidar system used. Statistics of the comparison between MWR- and reference lidar-based MLH retrievals show mean difference within 10 m, RMS within 340 m, and correlation coefficient higher than 0.77. Monthly mean analysis for day-time MLH from MWR, lidar, and radiosonde shows consistent seasonal variability, peaking at ~ 1200–1400 m in June and decreasing down to ~ 600 m in October. Conversely, night-time monthly mean MLH from all methods are within 300–500 m without any significant seasonal variability. The proposed method provides results that are more consistent with radiosonde estimates than MLH estimates from MWR retrieved profiles. MLH monthly mean values agree well within 1 std with bulk Richardson number method applied at radiosonde profiles at 11:00 and 23:00 UTC. The method described herewith operates continuously and it is expected to work with analogous performances for the entire diurnal cycle, except during considerable precipitation, demonstrating new potential for atmospheric observation by ground-based microwave radiometry.

Description: Stratospheric aerosol particle size information in Odin-OSIRIS limb scatter spectra Atmospheric Measurement Techniques Discussions, 6, 5065-5099, 2013 Author(s): L. A. Rieger, A. E. Bourassa, and D. A. Degenstein The Optical Spectrograph and InfraRed Imaging System (OSIRIS) on-board the Odin satellite has now taken over a decade of limb scatter measurements that have been used to retrieve the Version 5 stratospheric aerosol extinction product. This product is retrieved using a representative particle size distribution to calculate scattering cross sections and scattering phase functions for the forward model calculations. In this work the information content of OSIRIS measurements with respect to stratospheric aerosol is systematically examined for the purpose of retrieving particle size information along with the extinction coefficient. The benefit of using measurements at different wavelengths and scattering angles in the retrieval is studied and it is found that incorporation of the 1530 nm radiance measurement is key for a robust retrieval of particle size information. It is also found that using OSIRIS measurements at different solar geometries simultaneously provides little additional benefit. Based on these results, an improved aerosol retrieval algorithm is developed that couples the retrieval of aerosol extinction and mode radius of a log-normal particle size distribution. Comparison of these results with coincident measurements from SAGE III show agreement in retrieved extinction to within approximately 10% over the bulk of the aerosol layer, which is comparable to Version 5. The retrieved particle size, when converted to Ångström coefficient, shows good qualitative agreement with SAGE II measurements made at somewhat shorter wavelengths.

Description: SAGE version 7.0 algorithm: application to SAGE II Atmospheric Measurement Techniques Discussions, 6, 5101-5171, 2013 Author(s): R. P. Damadeo, J. M. Zawodny, L. W. Thomason, and N. Iyer This paper details the SAGE version 7.0 algorithm and how it is applied to SAGE II. Changes made between the previous (v6.2) and current (v7.0) versions are described and their impacts on the data products explained for both coincident event comparisons and time-series analysis. Users of the data will notice a general improvement in all of the SAGE II data products, which are now in better agreement with more modern data sets (e.g. SAGE III) and more robust for use with trend studies.

Description: Technical Note: Aeolian dust proxies produce visible luminescence upon intense laser-illumination that results from incandescence of internally mixed carbon Atmospheric Measurement Techniques Discussions, 6, 5173-5194, 2013 Author(s): L. Ma, T. Cao, and J. E. Thompson Mineral dust mimics dispersed in air produced visible luminescence between 550–800 nm when illuminated with a high peak power (MW range) Nd:YAG laser beam at 532 or 1064 nm. The luminescence persists for a few microseconds after the laser pulse and the measured emission spectrum is roughly consistent with a blackbody emitter at ≈4300 K. Both observations are consistent with assigning laser-induced incandescence (LII) as the source of the luminescence. However, light emission intensity from the mineral dust proxies is 240–4600 less intense than incandescence from fresh kerosene soot on a per-mass basis at laser pulse energies 90% on average. Heating to 350 °C reduced emission by 45–72%. Since black carbon soot and char (BC) oxidizes at elevated temperatures and BC is known to be present in soils, we conclude emission of light from the mineral dust aerosol proxies is likely a result of black carbon or char internally mixed within the soil dust sample. The reduction in LII response for samples heated to temperatures of 250–350 °C may result from partial oxidation of BC, but alternatively, could implicate a role for carbon present within organic molecules. The study suggests laser-induced incandescence measurements may allow quantitation of black carbon in soils and that soil dust is not truly an interferent in BC analysis by LII, but rather, a BC containing material.

Description: Retrieval of aerosol parameters from the oxygen A band in the presence of chlorophyll fluorescence Atmospheric Measurement Techniques Discussions, 6, 3181-3213, 2013 Author(s): A. F. J. Sanders and J. F. de Haan We have investigated precision of retrieved 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 noise using the forward model's derivatives. We assume that measurement noise is dominated by shot noise; thus, results apply to grating spectrometers in particular. In a number of retrieval simulations, we describe precision for various atmospheric states, observation geometries and spectral resolutions of the instrument. Our results show that aerosol optical thickness, aerosol pressure, fluorescence emission and surface albedo can be simultaneously retrieved from the O 2 A band. We also show that most of the fluorescence signal is provided by filling-in of the O 2 A band and to a lesser extent by filling-in of Fraunhofer lines.

Description: McClear: a new model estimating downwelling solar radiation at ground level in clear-sky conditions Atmospheric Measurement Techniques Discussions, 6, 3367-3405, 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. McClear implements a fully physical modelling replacing empirical relations or simpler models used before. It exploits the recent results on aerosol properties, and total column content in water vapor 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 tables, 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 in several stations within the Baseline Surface Radiation Network in various climates. For global, respectively direct, irradiance, the correlation coefficient ranges between 0.95 and 0.99, resp. 0.86 and 0.99. The bias is comprised between −14 and 25 W m −2 , resp. −49 and +33 W m −2 . The RMSE ranges between 20 W m −2 (3% of the mean observed irradiance) and 36 W m −2 (5%), resp. 33 W m −2 (5%) and 64 W m −2 (10%). These results are much better than those from state-of-the-art models. This work demonstrates the quality of the McClear model combined with MACC products, and indirectly the quality of the aerosol properties modeled by the MACC reanalysis.

Description: Experimental quantification of contact freezing in an electrodynamic balance Atmospheric Measurement Techniques Discussions, 6, 3407-3437, 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 an 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 allowing to determine the temperature dependent ice nucleation probability of size selected aerosol particles. The method uses supercooled charged water droplets suspended 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 time scale of our experiment.

Description: Separating mixtures of aerosol types in airborne High Spectral Resolution Lidar data Atmospheric Measurement Techniques Discussions, 6, 8269-8309, 2013 Author(s): S. P. Burton, M. A. Vaughan, R. A. Ferrare, and C. A. Hostetler Knowledge of aerosol type is important for source attribution and for determining the magnitude and assessing the consequences of aerosol radiative forcing. However, atmospheric aerosol is frequently not a single pure type, but instead occurs as a mixture of types, and this mixing affects the optical and radiative properties of the aerosol. This paper extends the work of earlier researchers by using the aerosol intensive parameters measured by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL-1) to develop a comprehensive and unified set of rules for characterizing the external mixing of several key aerosol intensive parameters: extinction-to-backscatter ratio (i.e. lidar ratio), backscatter color ratio, and depolarization ratio. We present the mixing rules in a particularly simple form that leads easily to mixing rules for the covariance matrices that describe aerosol distributions, rather than just scalar values of measured parameters. These rules can be applied to infer mixing ratios from the lidar-observed aerosol parameters, even for cases without significant depolarization. We demonstrate our technique with measurement curtains from three HSRL-1 flights which exhibit mixing between two aerosol types, urban pollution plus dust, marine plus dust, and smoke plus marine. For these cases, we infer a time-height cross-section of mixing ratio along the flight track, and partition aerosol extinction into portions attributed to the two pure types.

Description: Lidar-based remote sensing of atmospheric boundary layer height over land and ocean Atmospheric Measurement Techniques Discussions, 6, 8311-8338, 2013 Author(s): T. Luo, R. Yuan, and Z. Wang Atmospheric boundary layer (ABL) processes are important in climate, weather and air quality. A better understanding of the structure and the behavior of the ABL is required for understanding and modeling of the chemistry and dynamics of the atmosphere on all scales. Based on the systematic variations of ABL structures over different surfaces, different lidar-based methods were developed and evaluated to determine the boundary layer height and mixing layer height over land and ocean. With Atmospheric Radiation Measurement Program (ARM) Climate Research Facility (ACRF) micropulse lidar (MPL) and radiosonde measurements, diurnal and season cycles of atmospheric boundary layer depth and ABL vertical structure over ocean (TWP_C2 cite) and land (SGP_C1) are analyzed. The new methods are also applied to satellite lidar measurements. The derived global marine boundary layer structure database shows good agreement with marine ABL stratiform cloud top height.

Description: Fast reconstruction of hyperspectral radiative transfer simulations by using small spectral subsets: application to the oxygen A band Atmospheric Measurement Techniques Discussions, 6, 8339-8370, 2013 Author(s): A. Hollstein and R. Lindstrot Hyperspectral radiative transfer simulations are a versatile tool in remote sensing but can pose a major computational burden. We describe a simple method to construct hyperspectral simulation results by using only a small spectral subsample of the simulated wavelength range, thus leading to major speedups in such simulations. This is achieved by computing principal components for a small number of representative hyperspectral spectra and then deriving a reconstruction matrix for a specific spectral subset of channels to compute the hyperspectral data. The method is applied and discussed in detail using the example of top of atmosphere radiances in the oxygen A band, leading to speedups in the range of one to two orders of magnitude when compared to radiative transfer simulations at full spectral resolution.

Description: An assessment of cloud top thermodynamic phase products obtained from A-Train passive and active sensors Atmospheric Measurement Techniques Discussions, 6, 8371-8411, 2013 Author(s): S. Zeng, J. Riedi, F. Parol, C. Cornet, and F. Thieuleux The A-Train observations provide an unprecedented opportunity for the production of high quality dataset describing cloud properties. We illustrate in this study the use of one year of coincident POLDER (Polarization and Directionality of the Earth Reflectance), MODIS (MODerate Resolution Imaging Spectroradiometer) and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) observations to establish a reference dataset for the description of cloud top thermodynamic phase at global scale. We present the results of an extensive comparison between POLDER and MODIS cloud top phase products and discuss those in view of cloud vertical structure and optical properties derived simultaneously from collocated CALIOP active measurements. These results allow to identify and quantify potential biases present in the 3 considered dataset. Among those, we discuss the impacts of observation geometry, thin cirrus in multilayered and single layered cloud systems, supercooled liquid droplets, aerosols, fractional cloud cover and snow/ice or bright surfaces on global statistics of cloud phase derived from POLDER and MODIS passive measurements. Based on these analysis we define criteria for the selection of high confidence cloud phase retrievals which in turn can serve for the establishment of a reference cloud phase product. This high confidence joint product derived from POLDER/PARASOL and MODIS/Aqua can be used in the future as a benchmark for the evaluation of other cloud climatologies, for the assessment of cloud phase representation in models and the development of better cloud phase parametrization in the general circulation models (GCMs).

Description: Odin-OSIRIS detection of the Chelyabinsk meteor Atmospheric Measurement Techniques Discussions, 6, 8435-8443, 2013 Author(s): L. A. Rieger, A. E. Bourassa, and D. A. Degenstein On 15 February 2013 an 11 000 ton meteor entered Earth's atmosphere south east of Chelyabinsk creating a large fireball at 23 km altitude. The resulting stratospheric aerosol loading was detected by the Ozone Mapping and Profiler Suite (OMPS) in a high altitude polar belt. This work confirms the presence and lifetime of the stratospheric debris using the Optical Spectrograph and InfraRed Imaging System (OSIRIS) onboard the Odin satellite. Although OSIRIS coverage begins in mid-March, the measurements show a belt of enhanced scattering near 35 km altitude between 50° N and 70° N. Initially, enhancements show increased scattering of up to 15% over the background conditions, decaying in intensity and dropping in altitude until they are indistinguishable from background conditions by mid-May.

Description: Probabilistic approach to cloud and snow detection on AVHRR imagery Atmospheric Measurement Techniques Discussions, 6, 8445-8507, 2013 Author(s): J. P. Musial, F. Hüsler, M. Sütterlin, C. Neuhaus, and S. Wunderle The derivation of probability estimates complementary to geophysical data sets has gained special attention over the last years. The information about a confidence level of provided physical quantities is required to construct an error budget of higher level products and to correctly interpret final results of a particular analysis. Regarding the generation of products based on satellite data the common input consists of a cloud mask which allows discrimination between surface and cloud signals. Further the surface information is divided between snow and snow-free components. At any step of this discrimination process a misclassification in a cloud/snow mask propagates to higher level products and may alter their usability. Within this scope a novel Probabilistic Cloud Mask (PCM) algorithm suited for the 1×1 km Advanced Very High Resolution Radiometer (AVHRR) data is proposed which provides three types of probability estimates between: cloudy/clear-sky, cloudy/snow and clear-sky/snow conditions. As opposed to the majority of available techniques which are usually based on a decision-tree approach in the PCM algorithm all spectral, angular and ancillary information is used in a single step to retrieve the probability estimates from the pre-computed Look Up Tables (LUTs). Moreover, the issue of derivation of a single threshold value for a spectral test was overcome by the concept of multidimensional information space which is divided into small bins by an extensive set of thresholds. The discrimination between snow and ice clouds and detection of broken, thin clouds was enhanced by means of the Invariant Coordinate System (ICS) transformation. The study area covers a wide range of environmental conditions spanning from Iceland through central Europe to northern parts of Africa which exhibit diverse difficulties for cloud/snow masking algorithms. The retrieved PCM cloud classification was compared to the PPSv2012 and MOD35 collection 6 cloud masks, SYNOP weather reports, CALIPSO vertical feature mask version 3 and to MOD10A1 collection 5 snow mask. The outcomes of conducted analyses proved fine detection skills of the PCM method with comparable or better results than the reference PPS algorithm.

Description: Retrieval techniques for airborne imaging of methane concentrations using high spatial and moderate spectral resolution: application to AVIRIS Atmospheric Measurement Techniques Discussions, 6, 8543-8588, 2013 Author(s): A. K. Thorpe, C. Frankenberg, and D. A. Roberts Two quantitative retrieval techniques were evaluated to estimate methane (CH 4 ) enhancement in concentrated plumes using high spatial and moderate spectral resolution data from the Airborne Visible/Infrared Imaging Spectrometer (AVIRIS). An Iterative Maximum a Posteriori Differential Optical Absorption Spectroscopy (IMAP-DOAS) algorithm performed well for an ocean scene containing natural CH 4 emissions from the Coal Oil Point (COP) seep field near Santa Barbara, California. IMAP-DOAS retrieval precision errors are expected to equal between 0.31 to 0.61 ppm CH 4 over the lowest atmospheric layer (height up to 1.04 km), corresponding to about a 30 to 60 ppm error for a 10 m thick plume. However, IMAP-DOAS results for a terrestrial scene were adveresly influenced by the underlying landcover. A hybrid approach using Singular Value Decomposition (SVD) was particularly effective for terrestrial surfaces because it could better account for spectral variability in surface reflectance. Using this approach, a CH 4 plume was observed immediately downwind of two hydrocarbon storage tanks at the Inglewood Oil Field in Los Angeles, California, with a maximum near surface enhancement of 8.45 ppm above background. At COP, the distinct plume had a maximum enhancement of 2.85 ppm CH 4 above background and was consistent with known seep locations and local wind direction. A sensitivity analysis also indicates CH 4 sensitivity should be more than doubled for the next generation AVIRIS sensor (AVIRISng) due to improved spectral resolution and sampling. AVIRIS-like sensors offer the potential to better constrain emissions on local and regional scales, including sources of increasing concern like industrial point source emissions and fugitive CH 4 from the oil and gas industry.

Description: Effects of solar activity and geomagnetic field on noise in CALIOP profiles above the South Atlantic Anomaly Atmospheric Measurement Techniques Discussions, 6, 8589-8602, 2013 Author(s): V. Noel, H. Chepfer, C. Hoareau, M. Reverdy, and G. Cesana By documenting noise levels in 6.5 yr of nighttime measurements by the spaceborne lidar CALIOP above the South Atlantic Anomaly (SAA), we show they contain information about the evolution of upwelling high-energy radiation levels in the area. We find the amount of noisy profiles is influenced by the 11 yr cycle of solar activity, fluctuates by ±5% between 2006 and 2013, and is anticorrelated with solar activity with a 1 yr lag. The size of the SAA grows as solar activity decreases, and an overall westward shift of the SAA region is detectable. We predict SAA noise levels will increase anew after 2014, and will affect future spaceborne lidar missions most near 2020. In other areas, supposedly unaffected by incoming sunlight, nighttime noise levels are much weaker but follow the same 11 yr cycle, superimposed with a one-year cycle that affects both hemispheres similarly and could be attributed to geomagnetic activity.

Description: MODIS 3 km aerosol product: algorithm and global perspective Atmospheric Measurement Techniques Discussions, 6, 69-112, 2013 Author(s): L. A. Remer, S. Mattoo, R. C. Levy, and L. Munchak After more than a decade of producing a nominal 10 km aerosol product based on the dark target method, the MODIS aerosol team will be releasing a nominal 3 km product as part of their Collection 6 release. The new product differs from the original 10 km product only in the manner in which reflectance pixels are ingested, organized and selected by the aerosol algorithm. Overall, the 3 km product closely mirrors the 10 km product. However, the finer resolution product is able to retrieve over ocean closer to islands and coastlines, and is better able to resolve fine aerosol features such as smoke plumes over both ocean and land. In some situations, it provides retrievals over entire regions that the 10 km product barely samples. In situations traditionally difficult for the dark target algorithm, such as over bright or urban surfaces the 3 km product introduces isolated spikes of artificially high aerosol optical depth (AOD) that the 10 km algorithm avoids. Over land, globally, the 3 km product appears to be 0.01 to 0.02 higher than the 10 km product, while over ocean, the 3 km algorithm is retrieving a proportionally greater number of very low aerosol loading situations. Based on collocations with ground-based observations for only six months, expected errors associated with the 3 km land product are determined to be greater than for the 10 km product: ± 0.05 ± 0.25 AOD. Over ocean, the suggestion is for expected errors to be the same as the 10 km product: ± 0.03 ± 0.05 AOD. The advantage of the product is on the local scale, which will require continued evaluation not addressed here. Nevertheless, the new 3 km product is expected to provide important information complementary to existing satellite-derived products and become an important tool for the aerosol community.

Description: A comparison of rainfall measurements by multiple instruments Atmospheric Measurement Techniques Discussions, 6, 519-546, 2013 Author(s): X. C. Liu, T. C. Gao, and L. Liu Simultaneous observations of rainfall collected by a tipping bucket rain gauge, a weighing bucket rain gauge, an optical rain gauge, a present weather detector, a Joss–Waldvogel disdrometer, and a 2-D video disdrometer 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 in the order of 0 to 27.7%. The ORG, JWD, and 2DVD underestimated, and the TBRG overestimated the rain rate when R 〈 20 mm h −1 ; the TBRG agreed well with the reference values, while the PWD and 2DVD overestimated, WRG and JWD underestimated the rain rate when R 〉 20 mm h −1 . The TBRG and WRG underestimated more than 50% of rainfall duration substantially in the light rainfall, ORG underestimated the rainfall duration for about 12.7%, while the JWD and 2DVD overestimated the rainfall duration for more than 30%. The overall DSDs of JWD and 2DVD agreed well with each other, while the JWD had a higher volume mean diameter, lower raindrop numbers and liquid water content than that of 2DVD. The overestimation of small-size drops ( D 〈 1 mm) and underestimation of very large-size drops ( D 〉 4 mm) by JWD suggests the JWD's inaccuracy of measurement of small-size drops and very large-size drops; the underestimation of small raindrops by 2DVD suggested that DSDs in the heavy rainfall by 2DVD should be handled carefully.

Description: Ten years of MIPAS measurements with ESA Level 2 processor V6 – Part I: retrieval algorithm and diagnostics of the products Atmospheric Measurement Techniques Discussions, 6, 461-518, 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 instrument on the ENVISAT 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 processor, named ML2PP V6, 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 formalism 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 non-linear 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 2 O, O 3 , HNO 3 , CH 4 , N 2 O, 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: Polar night retrievals of trace gases in the Arctic using the Extended-range Atmospheric Emitted Radiance Interferometer Atmospheric Measurement Techniques Discussions, 6, 547-586, 2013 Author(s): Z. Mariani, K. Strong, M. Palm, R. Lindenmaier, C. Adams, X. Zhao, V. Savastiouk, C. T. McElroy, F. Goutail, and J. R. Drummond The Extended-range Atmospheric Emitted Radiance Interferometer (E-AERI) was installed at the Polar Environment Atmospheric Research Laboratory (PEARL) at Eureka, Nunavut, Canada in October 2008. Spectra from the E-AERI provide information about the radiative balance and budgets of trace gases in the Canadian high Arctic. Measurements are taken every seven minutes year-round, including polar night when the solar-viewing spectrometers at PEARL are not operated. This allows E-AERI measurements to fill the gap in the PEARL dataset during the four months of polar night. Measurements were taken year-round in 2008–2009 at the PEARL Ridge Lab, which is 610 m above sea-level, and from 2011-onwards at the Zero-Altitude PEARL Auxiliary Lab (0PAL), which is 15 km from the Ridge Lab at sea level. Total columns of O 3 , CO, CH 4 , and N 2 O have been retrieved using a modified version of the SFIT2 retrieval algorithm adapted for emission spectra. This provides the first nighttime measurements of these species at Eureka. Changes in the total columns driven by photochemistry and dynamics are observed. Analyses of E-AERI retrievals indicate accurate spectral fits (root-mean-square residuals 〈 1.5%) and a 10–15% uncertainty in the total column, depending on the trace gas. O 3 comparisons between the E-AERI and a Bruker IFS 125HR Fourier transform infrared (FTIR) spectrometer, three Brewer spectrophotometers, two UV-visible ground-based spectrometers, and a System D'Analyse par Observations Zenithales (SAOZ) at PEARL are made from 2008–2009 and for 2011. 125HR CO, CH 4 , and N 2 O columns are also compared with the E-AERI measurements. Mean relative differences between the E-AERI and the other spectrometers are 1–14% (depending on the gas), which are less than the E-AERI's total column uncertainties. The E-AERI O 3 and CO measurements are well correlated with the other spectrometers; the best correlation is with the 125HR ( r 〉 0.92). The 24-h diurnal cycle and 365-day seasonal cycle of CO are observed and their amplitudes are quantified by the E-AERI (6–12% and 46%, respectively). The seasonal variability of H 2 O has an impact on the retrievals, leading to larger uncertainties in the summer months. Despite increased water vapour at the lower-altitude site 0PAL, measurements at 0PAL are consistent with measurements at PEARL.

Description: Comparison of SMILES ClO profiles with other satellite and balloon-based measurements Atmospheric Measurement Techniques Discussions, 6, 613-663, 2013 Author(s): H. Sagawa, T. O. Sato, P. Baron, E. Dupuy, N. Livesey, J. Urban, T. von Clarmann, A. de Lange, G. Wetzel, 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 error analysis simulations 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 JAXA within of the bias uncertainties, except for the nighttime measurements in the low and middle latitude region 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, which makes it difficult to distinguish between the 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 datasets from other instruments such as the Aura Microwave Limb Sounder (MLS), the Odin Sub-Millimetre Radiometer (SMR), and the Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), 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 0.3 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 (MIPAS-B).

Description: Preliminary investigations toward nighttime aerosol optical depth retrievals from the VIIRS day/night band Atmospheric Measurement Techniques Discussions, 6, 587-612, 2013 Author(s): R. S. Johnson, J. Zhang, E. J. Hyer, S. D. Miller, and J. S. Reid A great need exists for reliable nighttime aerosol products at high spatial and temporal resolution. In this concept demonstration study, using Visible/Infrared Imager/Radiometer Suite (VIIRS) Day/Night Band (DNB) observations on the Suomi National Polar-orbiting Partnership (NPP) satellite, a new method is proposed for retrieving nighttime aerosol optical depth (τ) using the contrast between regions with and without artificial surface lights. Evaluation of the retrieved τ values against daytime AERONET data from before and after the overpass of the VIIRS satellite over the Cape Verde, Grand Forks, and Alta Floresta AERONET stations yields a coefficient of determination ( r 2 ) of 0.71. This study suggests that the VIIRS DNB has the potential to provide useful nighttime aerosol detection and property retrievals.

Description: Stack emission monitoring using non-dispersive infrared with optimized nonlinear absorption cross-interference correction algorithm Atmospheric Measurement Techniques Discussions, 6, 2009-2053, 2013 Author(s): Y.-W. Sun, C. Liu, K.-L. Chan, P.-H. Xie, W.-Q. Liu, Y. Zeng, S.-M. Wang, S.-H. Huang, J. Chen, Y.-P. Wang, and F.-Q. Si In this paper, we present an optimized analysis algorithm for non-dispersive infrared (NDIR) to monitor stack emissions. The newly developed analysis algorithm simultaneously compensates for nonlinear absorption and cross-interference between different gases. We present a mathematical derivation for the measurement error caused by variations in interference coefficients when nonlinear absorption occurs. The optimized algorithm is derived from a classical one and uses interference functions to quantify cross-interference. The interference functions vary proportionally with the nonlinear absorption. Thus, interference coefficients among different gases can be modeled by the interference functions whether gases are characterized by linear or nonlinear absorption. In this study, the simultaneous analysis of two components (CO 2 and CO) serves as an example for the validation of the optimized algorithm. The interference functions in this case can be obtained by least-squares fitting with three-order polynomials. Experiments show that the results of cross-interference correction are improved significantly by utilizing fitted interference functions when nonlinear absorptions occur. The dynamic measurement ranges of CO 2 and CO are improved by about a factor of 1.8 and 3.5, respectively. A commercial NDIR multi-gas analyzer with high accuracy was used to validate the CO and CO 2 measurements derived from the NDIR analyzer prototype in which the new cross-interference correction algorithm was embedded. Both measurements well agreed.

Description: Systematic residual ionospheric errors in radio occultation data and a potential way to minimize them Atmospheric Measurement Techniques Discussions, 6, 1979-2008, 2013 Author(s): J. Danzer, B. Scherllin-Pirscher, and U. Foelsche Radio Occultation (RO) sensing is used to probe the Earth's atmosphere in order to obtain information about its physical properties. With a main interest in the parameters of the neutral atmosphere, there is the need to perform a correction of the ionospheric contribution to the bending angle. Since this correction is an approximation to first order, there exists an ionospheric residual, which can be expected to be larger when the ionization is high (day versus night, high versus low solar activity). The ionospheric residual systematically affects the accuracy of the atmospheric parameters at low altitudes, at high altitudes (above 25 km to 30 km) it even is an important error source. In climate applications this could lead to a time dependent bias which induces wrong trends in atmospheric parameters at high altitudes. The first goal of our work was to study and characterize this systematic residual error. In a second step we developed a simple correction method, based purely on observational data, to reduce this residual for large ensembles of RO profiles. In order to tackle this problem we analyzed the bending angle bias of CHAMP and COSMIC RO data from 2001 to 2011. We could observe that the night time bending angle bias stays constant over the whole period of 11 yr, while the day time bias increases from low to high solar activity. As a result, the difference between night and day time bias increases from about −0.05 μrad to −0.4 μrad. This behavior paves the way to correct the solar cycle dependent bias of day time RO profiles. In order to test the newly developed correction method we performed a simulation study, which allowed to separate the influence of the ionosphere and the neutral atmosphere. Also in the simulated data we observed a similar increase in the bias in times from low to high solar activity. In this model world we performed the climatological ionospheric correction of the bending angle data, by using the bending angle bias characteristics of a solar cycle as a correction factor. After the climatological ionospheric correction the bias of the simulated data improved significantly, not only in the bending angle but also in the retrieved temperature profiles.

Description: Modified Ultrafast Thermometer UFT-M and temperature measurements during Physics of Stratocumulus Top (POST) Atmospheric Measurement Techniques Discussions, 6, 2085-2112, 2013 Author(s): W. Kumala, K. E. Haman, M. K. Kopec, D. Khelif, and S. P. Malinowski A modernised UFT-M version of the ultrafast airborne thermometer UFT was designed for the Physics of Stratocumulus Top (POST) field campaign. Improvements in its construction resulted in the sensor's increased reliability, which provided valuable measurements in 15 of the 17 flights. Oversampling the data allowed for the effective correction of the artefacts resulting from the interaction with the on-board avionic systems and the thermal noise resulting from the sensor construction. The UFT-M records, when averaged to the 1.4 m and 55 m resolutions, compared to the similar records of a thermometer in a Rosemount housing, indicate that the housing distorts even low-resolution airborne temperature measurements. Data collected with the UFT-M during the course of POST characterise the thermal structure of stratocumulus and capping inversion with the maximum resolution of ~ 1 cm. In this paper, examples of UFT-M records are presented and discussed.

Description: Towards a stable and absolute atmospheric carbon dioxide instrument using spectroscopic null method Atmospheric Measurement Techniques Discussions, 6, 2055-2083, 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 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: Rainfall measurement from opportunistic use of earth-space link in Ku Band Atmospheric Measurement Techniques Discussions, 6, 2113-2150, 2013 Author(s): L. Barthès and C. Mallet The present study deals with the development of a low cost microwave device devoted to measure average rain rate observed along earth – satellite links. The principle is to use rain atmospheric attenuation along Earth – space links in Ku-band to deduce the path averaged rain rate. These links are characterized by a path length of a few km through the troposphere. Ground based power measurements are carried out by receiving TV channels from different geostationary satellites in Ku-band. The major difficulty in this study is to retrieve rain characteristics among many fluctuations of the received signal which are due to atmospheric scintillations, changes in the composition of the atmosphere (water vapour concentration, cloud water content) or satellite features (variation of the emitted power, satellite motions). In order to perform a feasibility study of such a device, a measurement campaign has been performed for five months near Paris. This paper proposes an algorithm based on an artificial neural network to identify drought and rainy periods and to suppress the variability of the received signal due to no-rain effects. Taking into account the height of the rain layer, rain attenuation is then inverted to obtain path averaged rain rate. Obtained rainfall rates are compared with co-located rain gauges and radar measurements on the whole experiment period, then the most significant rainy events are analyzed.

Description: Performance of diethylene glycol based particle counters in the sub 3 nm size range Atmospheric Measurement Techniques Discussions, 6, 2151-2181, 2013 Author(s): D. Wimmer, K. Lehtipalo, A. Franchin, J. Kangasluoma, F. Kreissl, A. Kürten, A. Kupc, A. Metzger, J. Mikkilä, T. Petäjä, F. Riccobono, J. Vanhanen, M. Kulmala, and J. Curtius When studying new particle formation, the uncertainty in determining the "true" nucleation rate is considerably reduced when using Condensation Particle Counters (CPCs) capable of measuring concentrations of aerosol particles at sizes close to or even at the critical cluster size (1–2 nm). Recently CPCs, able to reliably detect particles below 2 nm in size and even close to 1 nm became available. The corrections needed to calculate nucleation rates are substantially reduced compared to scaling the observed formation rate to the nucleation rate at the critical cluster size. However, this improved instrumentation requires a careful characterization of their cut-off size and the shape of the detection efficiency curve because relatively small shifts in the cut-off size can translate into larger relative errors when measuring particles close to the cut-off size. Here we describe the development of two continuous flow CPCs using diethylene glycol (DEG) as the working fluid. The design is based on two TSI 3776 counters. Several sets of measurements to characterize their performance at different temperature settings were carried out. Furthermore two mixing-type Particle Size Magnifiers (PSM) A09 from Airmodus were characterized in parallel. One PSM was operated at the highest mixing ratio (1 L min −1 saturator flow), and the other was operated in a scanning mode, where the mixing ratios are changed periodically, resulting in a range of cut-off sizes. Different test aerosols were generated using a nano-Differential Mobility Analyzer (nano-DMA) or a high resolution DMA, to obtain detection efficiency curves for all four CPCs. One calibration setup included a high resolution mass spectrometer (APi-TOF) for the determination of the chemical composition of the generated clusters. The lowest cut-off sizes were achieved with negatively charged ammonium sulphate clusters, resulting in cut-offs of 1.4 nm for the laminar flow CPCs and 1.2 and 1.1 nm for the PSMs. A comparison of one of the laminar-flow CPCs and one of the PSMs measuring ambient and laboratory air showed good agreement between the instruments.

Description: Retrieval of aerosol optical depth over land surfaces from AVHRR data Atmospheric Measurement Techniques Discussions, 6, 2227-2251, 2013 Author(s): L. Mei, Y. Xue, A. A. Kokhanovsky, W. von Hoyningen-Huene, G. de Leeuw, and J. P. Burrows The Advanced Very High Resolution Radiometer (AVHRR) radiance data provide a global, long-term, consistent time series having high spectral and spatial resolution and thus being valuable for the retrieval of surface spectral reflectance, albedo and surface temperature. Long term time series of such data products are necessary for studies addressing climate change, sea ice distribution and movement, and ice sheet coastal configuration. These data have also been used to retrieve aerosol properties over ocean and land surfaces. However, the retrieval of aerosol over land and land surface albedo are challenging because of the information content of the measurement is limited and the inversion of these data products being ill defined. Solving the radiative transfer equations requires additional information and knowledge to reduce the number of unknowns. In this contribution we utilise an empirical linear relationship between the surface reflectances in the AVHRR channels at wavelengths of 3.75 μm and 2.1 μm, which has been identified in Moderate Resolution Imaging Spectroradiometer (MODIS) data. Next, following the MODIS dark target approach, the surface reflectance at 0.64 μm was obtained. The comparison of the estimated surface reflectance at 0.64 μm with MODIS reflectance products (MOD09) shows a strong correlation ( R = 0.7835). Once this was established, the MODIS "dark-target" aerosol retrieval method was adapted to Advanced Very High Resolution Radiometer (AVHRR) data. A simplified Look-Up Table (LUT) method, adopted from Bremen AErosol Retrieval (BAER) algorithm, was used in the retrieval. The Aerosol Optical Depth (AOD) values retrieved from AVHRR with this method compare favourably with ground-based measurements, with a correlation coefficient R = 0.861 and Root Mean Square Error (RMSE) = 0.17. This method can be easily applied to other satellite instruments which do not have a 2.1 μm channel, such as those currently planned to geostationary satellites.

Description: Enhancement of aerosol characterization using synergy of lidar and sun – photometer coincident observations: the GARRLiC algorithm Atmospheric Measurement Techniques Discussions, 6, 2253-2325, 2013 Author(s): A. Lopatin, O. Dubovik, A. Chaikovsky, Ph. Goloub, T. Lapyonok, D. Tanré, and P. Litvinov Currently most of experiments pursuing comprehensive characterization of atmosphere include coordinated observations by both lidar and radiometers in order to obtain important complimentary information about aerosol properties. The passive observations by radiometers from ground are mostly sensitive to the properties of aerosol in total atmospheric column and have very limited sensitivity to vertical structure of the atmosphere. Such observations are commonly used for measuring aerosol optical thickness and deriving the information about aerosol microphysics including aerosol particles shape, size distribution, and complex refractive index. In a contrast, lidar observations of atmospheric responses from different altitudes to laser pulses emitted from ground are designed to provide accurate profiling of the atmospheric properties. The interpretation of the lidar observation generally relies on some assumptions about aerosol type and loading. Here we present the GARRLiC algorithm (Generalized Aerosol Retrieval from Radiometer and Lidar Combined data) that simultaneously inverts co-incident lidar and radiometer observations and derives a united set of aerosol parameters. Such synergetic retrieval is expected to result in additional enhancements in derived aerosol properties because the backscattering observations by lidar add some sensitivity to the columnar properties of aerosol, while radiometric observations provide sufficient constraints on aerosol type and loading that generally are missing in lidar signals. GARRLiC is based on AERONET algorithm for inverting combined observations by radiometer and multi-wavelength elastic lidar observations. It is expected that spectral changes of backscattering signal obtained by multi-wavelength lidar at different altitudes provide some sensitivity to the vertical variability of aerosol particle sizes. In order to benefit from this sensitivity the algorithm is set to derive not only the vertical profile of total aerosol concentration but it also differentiates between the contributions of fine and coarse modes of aerosol. The detailed microphysical properties are assumed height independent and different for each mode and expected to be derived as a part of the retrieval. Thus, the GARRLiC inversion algorithm retrieves vertical distribution of both fine and coarse aerosol concentrations as well as the size distribution, complex refractive index and single scattering albedo for each mode. The potential and limitations of the method are demonstrated by the series of sensitivity tests. The practical outcome of the approach is illustrated by applications of the algorithm to the real lidar and radiometer observations obtained over selected AERONET site.

Description: Dimensionality reduction in Bayesian estimation algorithms Atmospheric Measurement Techniques Discussions, 6, 2327-2352, 2013 Author(s): G. W. Petty An idealized synthetic database loosely resembling 3-channel passive microwave observations of precipitation against a variable background is employed to examine the performance of a conventional Bayesian retrieval algorithm. For this dataset, algorithm performance is found to be poor owing to an irreconcilable conflict between the need to find matches in the dependent database versus the need to exclude inappropriate matches. It is argued that the likelihood of such conflicts increases sharply with the dimensionality of the observation space of real satellite sensors, which may utilize 9 to 13 channels to retrieve precipitation, for example. An objective method is described for distilling the relevant information content from N real channels into a much smaller number ( M ) of pseudochannels while also regularizing the background (geophysical plus instrument) noise component. The pseudochannels are linear combinations of the original N channels obtained via a two-stage principal component analysis of the dependent dataset. Bayesian retrievals based on a single pseudochannel applied to the independent dataset yield striking improvements in overall performance. The differences between the conventional Bayesian retrieval and reduced-dimensional Bayesian retrieval suggest that a major potential problem with conventional multichannel retrievals – whether Bayesian or not – lies in the common but often inappropriate assumption of diagonal error covariance. The dimensional reduction technique described herein avoids this problem by, in effect, recasting the retrieval problem in a coordinate system in which the desired covariance is lower-dimensional, diagonal, and unit magnitude.

Description: Aerosol retrieval experiments in the ESA Aerosol_cci project Atmospheric Measurement Techniques Discussions, 6, 2353-2411, 2013 Author(s): T. Holzer-Popp, G. de Leeuw, D. Martynenko, L. Klüser, S. Bevan, W. Davies, F. Ducos, J. L. Deuzé, R. G. Graigner, A. Heckel, W. von Hoyningen-Hüne, P. Kolmonen, P. Litvinov, P. North, C. A. Poulsen, D. Ramon, R. Siddans, L. Sogacheva, D. Tanre, G. E. Thomas, M. Vountas, J. Descloitres, J. Griesfeller, S. Kinne, M. Schulz, and S. Pinnock Within the ESA Climate Change Initiative (CCI) project Aerosol_cci (2010–2013) algorithms for the production of long-term total column aerosol optical depth (AOD) datasets from European Earth Observation sensors are developed. Starting with eight existing pre-cursor algorithms three analysis steps are conducted to improve and qualify the algorithms: (1) a series of experiments applied to one month of global data to understand several major sensitivities to assumptions needed due to the ill-posed nature of the underlying inversion problem, (2) a round robin exercise of "best" versions of each of these algorithms (defined using the step 1 outcome) applied to four months of global data to identify mature algorithms, and (3) a comprehensive validation exercise applied to one complete year of global data produced by the algorithms selected as mature based on the round robin exercise. The algorithms tested included four using AATSR, three using MERIS and one using PARASOL. This paper summarizes the first step. Three experiments were conducted to assess the potential impact of major assumptions in the various aerosol retrieval algorithms. In the first experiment a common set of four aerosol components was used to provide all algorithms with the same assumptions. The second experiment introduced an aerosol property climatology, derived from a combination of model and sun photometer observations, as a priori information in the retrievals on the occurrence of the common aerosol components and their mixing ratios. The third experiment assessed the impact of using a common nadir cloud mask for AATSR and MERIS algorithms in order to characterize the sensitivity to remaining cloud contamination in the retrievals against the baseline dataset versions. The impact of the algorithm changes was assessed for one month (September 2008) of data qualitatively by visible analysis of monthly mean AOD maps and quantitatively by comparing global daily gridded satellite data against daily average AERONET sun photometer observations for the different versions of each algorithm. The analysis allowed an assessment of sensitivities of all algorithms which helped define the best algorithm version for the subsequent round robin exercise; all algorithms (except for MERIS) showed some, in parts significant, improvement. In particular, using common aerosol components and partly also a priori aerosol type climatology is beneficial. On the other hand the use of an AATSR-based common cloud mask meant a clear improvement (though with significant reduction of coverage) for the MERIS standard product, but not for the algorithms using AATSR.

Description: A new stratospheric and tropospheric NO 2 retrieval algorithm for nadir-viewing satellite instruments: applications to OMI Atmospheric Measurement Techniques Discussions, 6, 1361-1407, 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 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 and are relatively free of modeling artifacts and negative tropospheric NO 2 values. In a re-analysis of an INTEX-B validation study, we show that SP2 largely eliminates a ∼20% discrepancy that existed between OMI and independent in situ springtime NO 2 SP1 measurements.

Description: Time series inversion of spectra from ground-based radiometers Atmospheric Measurement Techniques Discussions, 6, 1555-1588, 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 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: MISR Dark Water aerosol retrievals: operational algorithm sensitivity to particle non-sphericity Atmospheric Measurement Techniques Discussions, 6, 1589-1648, 2013 Author(s): O. V. Kalashnikova, M. J. Garay, J. V. Martonchik, and D. J. Diner The aim of this study is to theoretically investigate the sensitivity of the Multi-angle Imaging SpectroRadiometer (MISR) operational (Version 22) Dark Water retrieval algorithm to aerosol non-sphericity over the global oceans under actual observing conditions, accounting for current algorithm assumptions. Non-spherical (dust) aerosol models, which were introduced in Version 16 of the MISR aerosol product, improved the quality and coverage of retrievals in dusty regions. Due to the sensitivity of the retrieval to the presence of non-spherical aerosols, the MISR aerosol product has been successfully used to track the location and evolution of mineral dust plumes from the Sahara across the Atlantic, for example. However, the MISR global non-spherical aerosol optical depth (AOD) fraction product has been found to have several climatological artifacts superimposed on valid detections of mineral dust, including high non-spherical fraction in the Southern Ocean and seasonally variable bands of high non-sphericity. In this paper we introduce a formal approach to examine the ability of the operational MISR Dark Water algorithm to distinguish among various spherical and non-spherical particles as a function of the variable MISR viewing geometry. We demonstrate that under the criteria currently implemented: (1) Dark Water retrieval sensitivity to particle non-sphericity decreases for AOD below about 0.1 primarily due to an unnecessarily large lower bound imposed on the uncertainty in MISR observations at low light levels, and improves when this lower bound is removed; (2) Dark Water retrievals are able to distinguish between the spherical and non-spherical particles currently used for all MISR viewing geometries when the AOD exceeds 0.1; (3) the sensitivity of the MISR retrievals to aerosol non-sphericity varies in a complex way that depends on the sampling of the scattering phase function and the contribution from multiple scattering; and (4) non-sphericity artifacts occur at those view-illumination geometries where dust aerosols are indistinguishable from certain types of cirrus particles. Based on these results, we suggest that interested parties use caution with the Version 22 MISR Dark Water aerosol non-sphericity product in situations where cirrus may be present.

Description: MODIS 3 km aerosol product: applications over land in an urban/suburban region Atmospheric Measurement Techniques Discussions, 6, 1683-1716, 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 is including 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 data collected as part of the DISCOVER-AQ campaign; these data were measured by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL) and a network of 44 sun photometers (SP) spaced approximately 10 km apart. The HSRL instrument shows that AOD can vary by up to 0.2 within a single 10 km MODIS pixel, meaning that higher resolution satellite retrievals may help to 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 more than two-thirds of MODIS/SP collocations falling within the expected error envelope with high correlation ( R 〉 0.90). 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 significant 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: The Airborne Multiangle SpectroPolarimetric Imager (AirMSPI): a new tool for aerosol and cloud remote sensing Atmospheric Measurement Techniques Discussions, 6, 1717-1769, 2013 Author(s): D. J. Diner, F. Xu, M. J. Garay, J. V. Martonchik, B. E. Rheingans, S. Geier, A. Davis, B. R. Hancock, V. M. Jovanovic, M. A. Bull, K. Capraro, R. A. Chipman, and S. C. McClain The Airborne Multiangle SpectroPolarimetric Imager (AirMSPI) is an eight-band (355, 380, 445, 470, 555, 660, 865, 935 nm) pushbroom camera, measuring polarization in the 470, 660, and 865 nm bands, mounted on a gimbal to acquire multiangular observations over a ± 67° along-track range. The instrument has been flying aboard the NASA ER-2 high altitude aircraft since October 2010. AirMSPI employs a photoelastic modulator-based polarimetric imaging technique to enable accurate measurements of the degree and angle of linear polarization in addition to spectral intensity. A description of the AirMSPI instrument and ground data processing approach is presented. Example images of clear, hazy, and cloudy scenes over the Pacific Ocean and California land targets obtained during flights between 2010 and 2012 are shown, and quantitative interpretations of the data using vector radiative transfer theory and scene models are provided to highlight the instrument's capabilities for determining aerosol and cloud microphysical properties and cloud 3-D spatial distributions. Sensitivity to parameters such as aerosol particle size distribution, ocean surface wind speed and direction, cloud-top and cloud-base height, and cloud droplet size is discussed. AirMSPI represents a major step toward realization of the type of imaging polarimeter envisioned to fly on NASA's Aerosol-Cloud-Ecosystem (ACE) mission in the next decade.

Description: On the interference of 86 Kr 2+ during carbon isotope analysis of atmospheric methane using continuous flow combustion – isotope ratio mass spectrometry Atmospheric Measurement Techniques Discussions, 6, 1409-1460, 2013 Author(s): J. Schmitt, B. Seth, M. Bock, C. van der Veen, L. Möller, C. J. Sapart, M. Prokopiou, T. Sowers, T. Röckmann, and H. Fischer Stable carbon isotope analysis of methane (δ 13 C of CH 4 ) on atmospheric samples is one key method to constrain the current and past atmospheric CH 4 budget. A frequently applied measurement technique is gas chromatography isotope ratio mass spectrometry coupled to a combustion-preconcentration unit. This report shows that the atmospheric trace gas krypton can severely interfere during the mass spectrometric measurement leading to significant biases in δ 13 C of CH 4 if krypton is not sufficiently separated during the analysis. The effect comes about by the lateral tailing of the peak of doubly charged 86 Kr in the neighbouring m/z , 44, 45, and 46 Faraday cups. Accordingly, the introduced bias is dependent on the chromatographic separation, the Kr to CH 4 mixing ratio in the sample, the mass spectrometer source tuning as well as the detector configuration and can amount to up to several permil in δ 13 C. Apart from technical solutions to avoid this interference we present correction routines to a posteriori remove the bias.

Description: Aerosol classification from airborne HSRL and comparisons with the CALIPSO vertical feature mask Atmospheric Measurement Techniques Discussions, 6, 1815-1858, 2013 Author(s): S. P. Burton, R. A. Ferrare, M. A. Vaughan, A. H. Omar, R. R. Rogers, C. A. Hostetler, and J. W. Hair Aerosol classification products from the NASA Langley Research Center (LaRC) airborne High Spectral Resolution Lidar (HSRL-1) on the NASA B200 aircraft are compared with coincident V3.01 aerosol classification products from the CALIOP instrument on the CALIPSO satellite. For CALIOP, aerosol classification is a key input to the aerosol retrieval, and must be inferred using aerosol loading-dependent observations and location information. In contrast, HSRL-1 makes direct measurements of aerosol intensive properties, including the lidar ratio, that provide information on aerosol type. In this study, comparisons are made for 109 underflights of the CALIOP orbit track. We find that 62% of the CALIOP marine layers and 54% of the polluted continental layers agree with HSRL-1 classification results. In addition, 80% of the CALIOP desert dust layers are classified as either dust or dusty mix by HSRL-1. However, agreement is less for CALIOP smoke (13%) and polluted dust (35%) layers. Specific case studies are examined, giving insight into the performance of the CALIOP aerosol type algorithm. In particular, we find that the CALIOP polluted dust type is overused due to an attenuation-related depolarization bias. Furthermore, the polluted dust type frequently includes mixtures of dust plus marine aerosol. Finally, we find that CALIOP's identification of internal boundaries between different aerosol types in contact with each other frequently do not reflect the actual transitions between aerosol types accurately. Based on these findings, we give recommendations which may help to improve the CALIOP aerosol type algorithms.

Description: Detection of convective initiation using Meteosat SEVIRI: implementation in and verification with the tracking and nowcasting algorithm Cb-TRAM Atmospheric Measurement Techniques Discussions, 6, 1771-1813, 2013 Author(s): D. Merk and T. Zinner In this paper a new detection scheme for Convective Initation (CI) under day and night conditions is presented. The new algorithm combines the strengths of two existing methods for detecting Convective Initation with geostationary satellite data and uses the channels of the Spinning Enhanced Visible and Infrared Imager (SEVIRI) onboard Meteosat Second Generation (MSG). For the new algorithm five infrared criteria from the Satellite Convection Analysis and Tracking algorithm (SATCAST) and one High Resolution Visible channel (HRV) criteria from Cb-TRAM were adapted. This set of criteria aims for identifying the typical development of quickly developing convective cells in an early stage. The different criteria include timetrends of the 10.8 IR channel and IR channel differences as well as their timetrends. To provide the trend fields an optical flow based method is used, the Pyramidal Matching algorithm which is part of Cb-TRAM. The new detection scheme is implemented in Cb-TRAM and is verified for seven days which comprise different weather situations in Central Europe. Contrasted with the original early stage detection scheme of Cb-TRAM skill scores are provided. From the comparison against detections of later thunderstorm stages, which are also provided by Cb-TRAM, a decrease in false prior warnings (false alarm ratio) from 91 to 81% is presented, an increase of the critical success index from 7.4 to 12.7%, and a decrease of the BIAS from 320 to 146% for normal scan mode. Similar trends are found for rapid scan mode. Most obvious is the decline of false alarms found for synoptic conditions with upper cold air masses triggering convection.

Description: HelioFTH: combining cloud index principles and aggregated rating for cloud masking using infrared observations from geostationary satellites Atmospheric Measurement Techniques Discussions, 6, 1859-1898, 2013 Author(s): B. Dürr, M. Schröder, R. Stöckli, and R. Posselt A cloud mask, cloud fractional coverage (CFC) and cloud top pressure (CTP) retrieval scheme called HelioFTH is presented. The algorithm relies on infrared (IR) window channel observations only. The scheme is applicable to the full temporal and spatial resolution of the Meteosat Visible and InfraRed Imager (MVIRI) and the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) sensors. The main focus is laid on the separation of high cloud coverage (HCC) from low level clouds. CFC retrieval employs a IR-only cloud mask based on an aggregated rating scheme. CTP retrieval is based on a Heliosat-like cloud index for the MVIRI IR channel. CFC from HelioFTH, the International Satellite Cloud Climatology Project (ISCCP) DX and the Satellite Application Facility on Climate Monitoring (CM SAF) were validated with CFC from the Baseline Surface Radiation Network (BSRN) and the Alpine Surface Radiation Budget (ASRB) network. HelioFTH CFC differs by not more than 5–10% from CM SAF CFC but it is higher than ISCCP-DX CFC. In particular the conditional probability to detect cloud-free pixels with HelioFTH is raised by about 35% compared to ISCCP-DX. Also, the HelioFTH HCC was inter-compared to CM SAF and ISCCP-DX over different regions. The probability of false detection of cloud-free HCC pixels is 15% lower for HelioFTH than for ISCCP-DX compared to the CM SAF HCC product over the full-disk area. HelioFTH could be used for generating a climate data record of cloud physical properties once its consistency and homogeneity is validated for the full Meteosat time series.

Description: Absorbing aerosol radiative effects in the limb-scatter viewing geometry Atmospheric Measurement Techniques Discussions, 6, 1899-1942, 2013 Author(s): A. Wiacek, R. V. Martin, A. E. Bourassa, N. D. Lloyd, and D. A. Degenstein The limb-scatter satellite viewing geometry is well suited to detecting low-concentration aerosols in the upper troposphere due to its long observation path length (~ 50–100 km), high vertical resolution (~ 1–2 km) and good geographic coverage. We use the fully three-dimensional radiative transfer code SASKTRAN to simulate the sensitivity of limb-scatter viewing Odin/OSIRIS satellite measurements to absorbing mineral dust and carbonaceous aerosols (smoke and pure soot), as well as to non-absorbing sulfate aerosols and ice in the upper troposphere. At long wavelengths (813 nm) the addition of all aerosols (except soot) to an air only atmosphere produced a radiance increase as compared to air only, on account of the low Rayleigh scattering in air only at 813 nm. The radiance reduction due to soot aerosol was negligible ( 〈 0.1%) at all heights (0–100 km). At short wavelengths (337, 377, 452 nm), we found that the addition of any aerosol species to an air only atmosphere caused a decrease in single-scattered radiation due to an extinction of Rayleigh scattering in the direction of OSIRIS. The reduction was clearly related to particle size first, with absorption responsible for second-order effects only. Multiple-scattered radiation could either increase or decrease in the presence of an aerosol species, depending both on particle size and absorption. Large scatterers (ice, mineral dust) all increased multiple-scattered radiation within, below and above the aerosol layer. Small, highly absorbing pure soot particles produced a negligible multiple-scattering response ( 〈 0.1%) at all heights, primarily confined to within and below the soot layer. Medium-sized scatterers produced a multiple-scattering response that depended on their absorbing properties. Increased radiances were simulated as compared to air only at all short wavelengths (337, 377 and 452 nm) for sulfate aerosol particles (non-absorbing) while decreased radiances were simulated for smoke particles (absorbing) at 337 and 377 nm, where multiple scattering involving the medium-sized carbonaceous particles amplified their absorbing properties. At 452 nm, however, this effect was attenuated and albedo-dependent. At short wavelengths, the combined effect of single scattering decreases and multiple scattering increases led to complex total radiance signatures that generally could not unambiguously distinguish absorbing versus non-absorbing aerosols. Smoke aerosols led to a total radiance decrease (as compared to air only) at all altitudes above the aerosol layer (15–100 km). This unique signature was a result of the aerosols' strong absorbing properties, non-negligible scattering efficiency, and number concentrations high enough to make multiple scattering effects due to the aerosol itself significant. Thus, in the limb-scatter viewing geometry scene darkening above the aerosol layer is unambiguously due to absorption whereas scene darkening within and below the aerosol layer can simply be the result of a reduction in single-scattered radiance. Our simulations show a greater scene darkening for decreasing wavelengths, increasing surface albedo, decreasing solar zenith angle, and increasing particle number concentration, however, at 337 nm this effect did not exceed 0.2% of the total radiance due to air only, making the unique identification of medium-sized carbonaceous aerosols, i.e. smoke, difficult. Scene darkening (or brightening) varies linearly with particle number concentration over three orders of magnitude. A fortuitous, unexpected implication of our analysis is that limb-scatter retrievals of aerosol extinction are insensitive to external information about aerosol absorption.

Description: Validation of middle atmospheric campaign-based water vapour measured by the ground-based microwave radiometer MIAWARA-C Atmospheric Measurement Techniques Discussions, 6, 1311-1359, 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 way 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). MIAWARA-C measures two polarisations of the incident radiation in separate receiver channels and can therefore provide two independent measurements of the same air mass. The standard deviation of the difference between the profiles obtained from the two polarisations is in excellent agreement with the estimated random error of v1.1. In this paper, the quality of v1.1 data is assessed during two measurement campaigns: (1) five 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 campaigns 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-latitudinal campaign. In general all intercomparisons show high correlation coefficients, above 0.5 at altitudes above 45 km, confirming the ability of MIAWARA-C to monitor temporal variations on the order of days. The biases are generally below 10% 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.

Description: CO 2 , CO and CH 4 measurements from the NOAA Earth System Research Laboratory's Tall Tower Greenhouse Gas Observing Network: instrumentation, uncertainty analysis and recommendations for future high-accuracy greenhouse gas monitoring efforts Atmospheric Measurement Techniques Discussions, 6, 1461-1553, 2013 Author(s): A. E. Andrews, J. D. Kofler, M. E. Trudeau, J. C. Williams, D. H. Neff, K. A. Masarie, D. Y. Chao, D. R. Kitzis, P. C. Novelli, C. L. Zhao, E. J. Dlugokencky, P. M. Lang, M. J. Crotwell, M. L. Fischer, M. J. Parker, J. T. Lee, D. D. Baumann, A. R. Desai, C. O. Stanier, S. F. J. de Wekker, D. E. Wolfe, J. W. Munger, and P. P. Tans A robust in situ CO 2 and CO analysis system has been developed and deployed at eight sites in the NOAA Earth System Research Laboratory's (ESRL) Tall Tower Greenhouse Gas Observing Network. The network uses very tall (〉 300 m) television and radio transmitter towers that provide a convenient platform for mid-boundary layer trace gas sampling. Each analyzer has three sample inlets for profile sampling, and a complete vertical profile is obtained every 15 min. The instrument suite at one site has been augmented with a cavity ring-down spectrometer for measuring CO 2 and CH 4 . The long-term stability of the systems in the field is typically better than 0.1 ppm for CO 2 , 6 ppb for CO, and 0.5 ppb for CH 4 , as determined from repeated standard gas measurements. The instrumentation is fully automated and includes sensors for measuring a variety of status parameters, such as temperatures, pressures and flow rates that are inputs for automated alerts and quality control algorithms. These algorithms provide detailed and time-dependent uncertainty estimates for all of the gases and could be adapted to other species or analysis systems. The design emphasizes use of off the shelf parts and modularity to facilitate network operations and ease of maintenance. The systems report high-quality data with 〉 93% uptime. Recurrent problems and limitations of the current system are discussed along with general recommendations for high accuracy trace-gas monitoring. The network is a key component of the North American Carbon Program and a useful model for future research-grade operational greenhouse gas monitoring efforts.

Description: Development of a neural network model for cloud fraction detection using NASA-Aura OMI VIS radiance measurements Atmospheric Measurement Techniques Discussions, 6, 1649-1681, 2013 Author(s): G. Saponaro, P. Kolmonen, J. Karhunen, J. Tamminen, and G. de Leeuw The discrimination of cloudy pixels is required in almost any estimate of a parameter retrieved from a satellite image in the ultraviolet (UV), visual (VIS) or infra-red (IR) parts of the electromagnetic spectrum. Also, the distincion of clouds within satellite imagery and the distribution of their micro-physical properties is essential to the understanding of radiative transfer through the atmosphere. This paper reports the development of neural network algorithms for cloud detection for the NASA-Aura Ozone Monitoring Instrument (OMI). We present and discuss the results obtained by training mathematical neural networks with simultaneous application to OMI and Aqua-MODerate Resolution Imaging Spectrometer (MODIS) data. The neural network delivers cloud fraction estimates in a fast and automated way. The developed neural network approach performs generally well in the training. Highly reflective surfaces, such as ice, snow, sun glint and desert, or atmospheric dust mislead the neural network to a wrong predicted cloud fraction.

Description: Retrieving wind statistics from average spectrum of continuous-wave lidar Atmospheric Measurement Techniques Discussions, 6, 1943-1977, 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 lidar is proportional to the probability density function of the line-of-sight velocities. This would open the possibility of using cw lidars for a precise 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.

Description: Validation of the METEOSAT storm detection and nowcasting system Cb-TRAM with lightning network data – Europe and South Africa Atmospheric Measurement Techniques Discussions, 6, 1269-1310, 2013 Author(s): T. Zinner, C. Forster, E. de Coning, and H.-D. Betz In this manuscript, recent changes to the DLR METEOSAT thunderstorm TRacking And Monitoring algorithm (Cb-TRAM) are presented as well as a validation of Cb-TRAM against the European ground-based LIghtning NETwork data (LINET) of Nowcast GmbH and Lightning Detection Network (LDN) data of the South African Weather Service (SAWS). The validation is conducted along the well known skill scores probability of detection (POD) and false alarm ratio (FAR) on the basis of METEOSAT/SEVIRI pixels as well as on the basis of thunderstorm objects. The values obtained demonstrate the limits of Cb-TRAM in specific as well as the limits of satellite methods in general which are based on thermal emission and solar reflectivity information from thunderstorm tops. Although the climatic conditions and the occurence of thunderstorms is quite different for Europe and South Africa, the quality score values are similar. Our conclusion is that Cb-TRAM provides robust results of well-defined quality for very different climatic regimes. The POD for a thunderstorm with intense lightning is about 80% during the day. The FAR for a Cb-TRAM detected thunderstorm which is not at least close to intense lightning activity is about 50%; if the proximity to any lightning activity is evaluated the FAR is even much lower at about 15%. Pixel-based analysis shows that the detected thunderstorm object size is not indiscriminately large, but well within the physical limitations of the method. Nighttime POD and FAR are somewhat worse as the detection scheme can not use high resolution visible information. Nowcasting scores show useful values up to approximatelly 30 min.

Description: Assessment of the CALIPSO Lidar 532 nm version 3 lidar ratio models using a ground-based lidar and AERONET sun photometers in Brazil Atmospheric Measurement Techniques Discussions, 6, 1143-1199, 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 two ground-based remote sensing instruments: a single elastic backscatter lidar system and the AERONET sun photometers installed at five different locations in Brazil. In this study we develop a validation methodology to assess 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 ratio values determined from the combination of AERONET optical depth measurements and CALIOP integrated attenuated backscatter show good agreement with the model values assigned by the CALIOP algorithm. These comparisons yield a mean percentage difference of −2% ± 26%. Similarly, lidar ratio values retrieved by the elastic backscatter lidar system at IPEN show a mean percentage difference of −2% ± 15% when compared with CALIOP's lidar ratio. These results confirm the accuracy in the lidar ratio estimates provided by the CALIOP algorithms to within an uncertainty range of no more than 30%.

Description: On the optimal method for evaluating cloud products from passive satellite imagery using CALIPSO-CALIOP data: example investigating the CM SAF CLARA-A1 dataset Atmospheric Measurement Techniques Discussions, 6, 1093-1141, 2013 Author(s): K.-G. Karlsson and E. Johansson A method for detailed evaluation of a new satellite-derived global 28-yr cloud and radiation climatology (Climate Monitoring SAF Cloud, Albedo and Radiation dataset from AVHRR data, named CLARA-A1) from polar orbiting NOAA and Metop satellites is presented. The method combines 1 km and 5 km resolution cloud datasets from the CALIPSO-CALIOP cloud lidar for estimating cloud detection limitations and the accuracy of cloud top height estimations. Cloud detection is shown to work efficiently for clouds with optical thicknesses above 0.30 except for at twilight conditions when this value increases to 0.45. Some misclassifications generating erroneous clouds over land surfaces in semi-arid regions in the sub-tropical and tropical regions are revealed. In addition, a substantial fraction of all clouds remains undetected in the Polar regions during the polar winter season due to the lack of or an inverted temperature contrast between Earth surfaces and clouds. Subsequent cloud top height evaluation took into account the derived information about the cloud detection limits. It was shown that this has fundamental importance for the achieved results. An overall bias of −274 m was achieved compared to a bias of −2762 m if no measures were taken to compensate for cloud detection limitations. Despite this improvement it was concluded that high-level clouds still suffer from substantial height underestimations while the opposite is true for low-level (boundary layer) clouds. The validation method and the specifically collected satellite dataset with optimal matching in time and space are suggested for a wider use in the future for evaluation of other cloud retrieval methods based on passive satellite imagery.

Description: Airborne emission measurements of SO 2 , NO x and particles from individual ships using sniffer technique Atmospheric Measurement Techniques Discussions, 6, 10617-10651, 2013 Author(s): J. Beecken, J. Mellqvist, K. Salo, J. Ekholm, and J.-P. Jalkanen A dedicated system for airborne ship emission measurements of SO 2 , NO x and particles has been developed and used from several small aircrafts. The system has been adapted for fast response measurements at 1 Hz and the use of several of the instruments is unique. The uncertainty of the given data is about 20.3% for SO 2 and 23.8% for NO x emission factors. Multiple measurements of 158 ships measured from the air on the Baltic and North Sea during 2011 and 2012 show emission factors of 18.8 ± 6.5 g kg fuel −1 , 66.6 ± 23.4 g kg fuel −1 , and 1.8 ± 1.3 × 10 16 particles kg fuel −1 for SO 2 , NO x and particle number respectively. The particle size distributions were measured for particle diameters between 15 and 560 nm. The mean sizes of the particles are between 50 and 62 nm dependent on the distance to the source and the number size distribution is mono-modal. Concerning the sulfur fuel content 85% of the ships comply with the IMO limits. The sulfur emission has decreased compared to earlier measurements from 2007 to 2009. The presented method can be implemented for regular ship compliance monitoring.

Description: Multi-modal analysis of aerosol robotic network size distributions for remote sensing applications: dominant aerosol type cases Atmospheric Measurement Techniques Discussions, 6, 10571-10615, 2013 Author(s): M. Taylor, S. Kazadzis, and E. Gerasopoulos To date, size distributions obtained from the aerosol robotic network have been fit with bi-lognormals defined by six secondary microphysical parameters: the volume concentration, effective radius, and the variance of fine and coarse particle modes. However, since the total integrated volume concentration is easily calculated and can be used as an accurate constraint, the problem of fitting the size distribution can be reduced to that of deducing a single free parameter – the mode separation point. We present a method for determining the mode separation point for equivalent-volume bi-lognormal distributions based on optimisation of the root mean squared error and the coefficient of determination. The extracted secondary parameters are compared with those provided by AERONET's Level 2.0 Version 2 inversion algorithm for a set of benchmark dominant aerosol types including: desert dust, biomass burning aerosol, urban sulphate and sea salt. The total volume concentration constraint is then also lifted by performing multi-modal fits to the size distribution using nested Gaussian mixture models and a method is presented for automating the selection of the optimal number of modes using a stopping condition based on Fisher statistics and via the application of statistical hypothesis testing. It is found that the method for optimizing the location of the mode separation point is independent of the shape of the AVSD, does not require the existence of a local minimum in the size interval 0.439 μm ≤ r ≤ 0.992 μm, and shows some potential for optimizing the bi-lognormal fitting procedure used by AERONET particularly in the case of desert dust aerosol. The AVSD of impure marine aerosol is found to require 3 modes. In this particular case, bi-lognormals fail to recover key features of the AVSD. Fitting the AVSD more generally with multi-modal models allows automatic detection of a statistically-significant number of aerosol modes, is applicable to a very diverse range of aerosol types, and gives access to the secondary microphysical parameters of additional modes currently not available from bi-lognormal fitting methods.

Description: A concept of an automated function control for ambient aerosol measurements using mobility particle size spectrometers Atmospheric Measurement Techniques Discussions, 6, 10551-10570, 2013 Author(s): A. Schladitz, M. Merkel, S. Bastian, W. Birmili, K. Weinhold, G. Löschau, and A. Wiedensohler An automated function control unit was developed to regularly check the ambient particle number concentration derived from a mobility particle size spectrometer as well as its zero-point behaviour. The aim of the new feature is to conduct unattended quality control experiments under field conditions at remote air quality monitoring or research stations. The automated function control also has the advantage of being able to get a faster system stability response than the recommended on-site comparisons with reference instruments. The method is based on a comparison of the total particle number concentration measured by a mobility particle size spectrometer and a condensation particle counter removing the diffusive particles approximately smaller than 25 nm in diameter. In practice, the small particles are removed by a set of diffusion screens, as traditionally used in a diffusion battery. The other feature of the automated function control is to check the zero-point behaviour of the ambient aerosol passing through a high-efficiency particulate air (HEPA) filter. An exemplary one-year data set is presented for the measurement site Annaberg-Buchholz as part of the Saxon air quality monitoring network. The total particle number concentration derived from the mobility particle size spectrometer overestimates the particle number concentration by only 2% (grand average offset). Furthermore, tolerance criteria are presented to judge the performance of the mobility particle size spectrometer with respect to the particle number concentration. An upgrade of a mobility particle size spectrometer with an automated function control enhances the quality of long-term particle number size distribution measurements. Quality assured measurements are a precondition for intercomparison studies of different sites. Comparable measurements will improve cohort health and also climate-relevant research studies.

Description: The mobile Water vapor Aerosol Raman LIdar and its implication in the frame of the HyMeX and ChArMEx programs: application to a dust transport process Atmospheric Measurement Techniques Discussions, 6, 10653-10698, 2013 Author(s): P. Chazette, F. Marnas, and J. Totems The increasing importance of the coupling of water and aerosol cycles in environmental applications requires observation tools which allow simultaneous measurements of these two fundamental processes for climatological and meteorological studies. In this purpose, a new mobile Raman lidar, WALI (Water vapor and Aerosol LIDAR), has been developed and implemented within the framework of the international HyMeX/IODA-MED and ChArMEx programs. This paper presents the key properties of this new device and its first applications to scientific studies. The lidar uses an eye-safe emission in the ultra-violet range at 354.7 nm and a set of compact refractive receptors. Cross-comparisons between rawindsoundings performed from balloon or aircraft and lidar measurements have shown a good agreement in the derived water vapor mixing ratio (WVMR). The discrepancies are generally less than 0.5 g kg −1 and therefore within the error bars of the instruments. A detailed study of the uncertainties was conducted and shows a 7 to 11% accuracy of the WVMR retrieval, which is largely constrained by the quality of the calibration. It also proves that the lidar is able to measure the WVMR during the day over a range of about 1 km. The WALI system otherwise provides measurements of aerosol optical properties such as the lidar ratio (LR) or the particulate depolarization ratio (PDR). An important example of scientific application addressing the main objectives of the HyMeX and ChArMEx programs is then presented, following an event of desert dust aerosols over the Balearic Islands. This dust intrusion may have had a significant impact on the intense precipitations that occurred over southwestern France and the Spanish Mediterranean coasts. During this event, the LR and PDR values obtained are in the ranges of ~ 45–63 ± 6 sr and 0.1–0.19 ± 0.01, respectively, which is representative of dust aerosols. The dust layers are also shown to be associated with significant WVMR, i.e. between 4 and 6.7 g kg −1 .

Description: Aerosol seasonal variations over urban sites in Ukraine and Belarus according to AERONET and POLDER measurements Atmospheric Measurement Techniques Discussions, 6, 10731-10759, 2013 Author(s): G. Milinevsky, V. Danylevsky, V. Bovchaliuk, A. Bovchaliuk, Ph. Goloub, O. Dubovik, V. Kabashnikov, A. Chaikovsky, M. Mishchenko, and M. Sosonkin The paper presents an investigation of aerosol seasonal variations in several urban sites in the East European region. Our analysis of seasonal variations of optical and physical aerosol parameters is based on the sun-photometer 2008–2012 data from three urban ground-based AERONET sites in Ukraine (Kyiv, Kyiv-AO, and Lugansk) and one site in Belarus (Minsk), as well as on satellite POLDER instrument data for urban areas in Ukraine. Aerosol amount and optical thickness values exhibit peaks in the spring (April–May) and late summer (August), whereas minimum values are seen in late autumn over the Kyiv and Minsk sites. The results show that aerosol fine mode particles are most frequently detected during the spring and late summer seasons. The seasonal variation similarity in the two regions points to the resemblance in basic aerosol sources which are closely related to properties of aerosol particles. However the aerosol amount and properties change noticeably from year to year and from region to region. The analysis of seasonal aerosol optical thickness variations over the urban sites in the eastern and western parts of Ukraine according to both ground-based and POLDER data exhibits the same traits. In particular, over Kyiv, the values of the Angstrom exponent are lower in April of 2011 than in 2009 and 2010, while aerosol optical thickness values are almost the same, which can be explained by an increase in the amount of coarse mode particles in the atmosphere, such as Saharan dust. Moreover, the coarse mode particles prevailed over suburbs and the center of Kyiv during a third of all available days of observation in 2012. In general, the fine and coarse mode particles' modal radii averaged over 2008–2012 range from 0.1 to 0.2 μm and 2 to 5 μm, respectively, during the period from April to September. The single scattering albedo and refractive index values of these particles correspond to a mix of urban-industrial, biomass burning, and dust aerosols. In addition, strongly absorbing particles were observed in the period from October to March, and the modal radius of fine and coarse mode particles changed from month to month widely.

Description: Aerosol optical properties in Northern Norway and Svalbard Atmospheric Measurement Techniques Discussions, 6, 10761-10795, 2013 Author(s): Y.-C. Chen, B. Hamre, Ø. Frette, S. Blindheim, K. Stebel, P. Sobolewski, C. Toledano, and J. J. Stamnes We present comparisons between estimates of the aerosol optical thickness and the Ångström exponent in Northern Norway and Svalbard based on data from AERONET (Aerosol Robotic Network) stations at Andenes (69.28° N, 16.01° E, 379 m altitude) and Hornsund (77.00° N, 15.56° E, 10 m altitude) for the period 2008–2011. The four-year annual mean values for the aerosol optical thickness at 500 nm τ(500) at Andenes and Hornsund both were 0.10. At Hornsund, there was less variation of the monthly mean value of τ(500) than at Andenes. The annual mean values of the Ångström exponent α at Andenes and Hornsund were 1.25 and 1.37, respectively. At Andenes and Hornsund α was found to be larger than 1.1 in 64% and 86% of the observations, respectively, indicating that fine-mode particles were dominating at both sites. Both sites had a similar seasonal variation of the aerosol size distribution although one site is in an arctic area while the other site is in a sub-arctic area.

Description: The detectability of nitrous oxide mitigation efficacy in intensively grazed pastures using a multiple plot micrometeorological technique Atmospheric Measurement Techniques Discussions, 6, 8959-9003, 2013 Author(s): A. M. S. McMillan, M. J. Harvey, R. J. Martin, A. M. Bromley, M. J. Evans, S. Mukherjee, and J. Laubach Methodologies are required to verify agricultural greenhouse gas mitigation at scales relevant to farm management. Micrometeorological techniques provide a viable approach for comparing fluxes between fields receiving mitigation treatments and control fields. However, they have rarely been applied to spatially verifying treatments aimed at mitigating nitrous oxide emission from intensively grazed pastoral systems. We deployed a micrometeorological system to compare N 2 O flux among several ~ 1.5 ha plots in intensively grazed dairy pasture. The sample collection and measurement system is referred to as the Field-Scale Nitrous Oxide Mitigation Assessment System (FS-NOMAS) and used a tuneable diode laser absorption spectrometer to measure N 2 O gradients to high precision at four locations along a 300 m transect. The utility of the FS-NOMAS to assess mitigation efficacy depends largely on its ability to resolve very small vertical N 2 O gradients. The performance of the FS-NOMAS was assessed in this respect in laboratory and field-based studies. The FS-NOMAS could reliably resolve gradients of 0.039 ppb between a height of 0.5 m and 1.0 m. The gradient resolution achieved corresponded to the ability to detect an inter-plot N 2 O flux difference of 26.4 μg N 2 O-N m −2 h −1 under the most commonly encountered conditions of atmospheric mixing (quantified here by a turbulent transfer coefficient), but this ranged from 11 to 59 μg N 2 O-N m −2 h −1 as the transfer coefficient ranged between its 5th and 95th percentile. Assuming a likely value of 100 μg N 2 O-N m −2 h −1 for post-grazing N 2 O fluxes from intensively grazed New Zealand dairy pasture, the system described here would be capable of detecting a mitigation efficacy of 26% for a single (40 min) comparison. We demonstrate that the system has considerably greater sensitivity to treatment effects by measuring cumulative fluxes over extended periods.

Description: Near-infrared remote sensing of Los Angeles trace gas distributions from a mountaintop site Atmospheric Measurement Techniques Discussions, 6, 8807-8854, 2013 Author(s): D. Fu, T. J. Pongetti, J.-F. L. Blavier, T. J. Crawford, K. S. Manatt, G. C. Toon, K. W. Wong, and S. P. Sander The Los Angeles basin is a significant anthropogenic source of major greenhouse gases (CO 2 and CH 4 ) and the pollutant CO, contributing significantly to regional and global climate change. We present a novel approach for monitoring the spatial and temporal distributions of greenhouse gases in the Los Angeles basin using a high-resolution spectroscopic remote sensing technique. A new Fourier Transform Spectrometer called CLARS-FTS has been deployed since May 2010 at JPL's California Laboratory for Atmospheric Remote Sensing (CLARS) on Mt. Wilson, California for automated long-term measurements of greenhouse gases. The instrument design and performance of CLARS-FTS are presented. From its mountaintop location at an altitude of 1673 m, the instrument points at a programmed sequence of ground target locations in the Los Angeles basin, recording spectra of reflected near-IR solar radiation. Column-averaged dry-air mole fractions of greenhouse gases (XGHG) including XCO 2 , XCH 4 , and XCO are retrieved several times per day for each target. Spectra from a local Spectralon® scattering plate are also recorded to determine background (free tropospheric) column abundances above the site. Comparisons between measurements from LA basin targets and the Spectralon® plate provide estimates of the boundary layer partial column abundances of the measured species. Algorithms are described for transforming the measured interferograms into spectra, and for deriving column abundances from the spectra along with estimates of the measurement precision and accuracy. The CLARS GHG measurements provide a means to infer relative, and possibly absolute, GHG emissions.

Description: Net ecosystem CO 2 exchange measurements by the closed chamber method and the eddy covariance technique and their dependence on atmospheric conditions – a case study Atmospheric Measurement Techniques Discussions, 6, 8783-8805, 2013 Author(s): M. Riederer, A. Serafimovich, and T. Foken Carbon dioxide flux measurements in ecosystem sciences are mostly conducted by eddy covariance technique or the closed chamber method. Also some comparisons have been performed. But there is a lack of detailed assessment of present differences and uncertainties. To determine underlying processes, a ten-day, side-by-side measurement of the net ecosystem exchange with both techniques was evaluated with regard to various atmospheric conditions during the diurnal cycle. It was found that, depending on the particular atmospheric condition, the chamber carbon dioxide flux was either: (i) equal to the carbon dioxide flux measured by the reference method eddy covariance, by day with well developed atmospheric turbulence, (ii) higher, in the afternoon in times of oasis effect, (iii) lower, predominantly at night while large coherent structure fluxes or high wind velocities prevailed, or, (iv) showed less variation in the flux pattern, at night while stable stratification was present. Due to lower chamber carbon dioxide fluxes at night, when respiration forms the net ecosystem exchange, and higher chamber carbon dioxide fluxes in the afternoon, when the ecosystem is still a net carbon sink, there are two complementary aspects resulting in an overestimation of the ecosystem sink capacity by the chamber of 40% in this study.

Description: Sub 3 nm particle size and composition dependent response of a nano-CPC battery Atmospheric Measurement Techniques Discussions, 6, 8855-8887, 2013 Author(s): J. Kangasluoma, C. Kuang, D. Wimmer, M. P. Rissanen, K. Lehtipalo, M. Ehn, D. R. Worsnop, J. Wang, M. Kulmala, and T. Petäjä In this study we built a nano-CPC battery, consisting of four ultrafine CPCs optimized for the detection of sub 3 nm particles. Two of the CPCs use diethylene glycol as a working fluid: a laminar type diethlylene glycol CPC and a mixing type Airmodus A09 Particle Size Magnifier. The other two CPCs are a laminar type TSI 3025A and a TSI 3786 with butanol and water as the working fluids, respectively. The nano-CPC battery was calibrated with seven different test aerosols: tetra heptyl ammonium bromide, ammonium sulphate, sodium chloride, tungsten oxide, sucrose, candle flame products and limonene ozonolysis products. The results show that ammonium sulphate and sodium chloride have a higher activation efficiency with the water-based 3786 than with the butanol-based 3025A, whereas the other aerosols were activated better with butanol than with water as the working fluid. It is worthwhile to mention that limonene ozonolysis products were detected very poorly with all of the CPCs, butanol being the best fluid to activate the oxidation products. To explore how the detection efficiency is affected if the aerosol is an internal mixture of two different chemical substances, we made the first attempt to control the mixing state of sub 3 nm laboratory generated aerosol. We show that we generated an internally mixed aerosol of ammonium sulphate nucleated onto tungsten oxide seed particles, and observed that the activation efficiency of the internally mixed clusters was a function of the internal mixture composition.

Description: Volcanic ash infrared signature: realistic ash particle shapes compared to spherical ash particles Atmospheric Measurement Techniques Discussions, 6, 8937-8958, 2013 Author(s): A. Kylling, M. Kahnert, H. Lindqvist, and T. Nousiainen The reverse absorption technique is often used to detect volcanic clouds from thermal infrared satellite measurements. From these measurements particle size and mass loading may also be estimated using radiative transfer modelling. The radiative transfer modelling usually assumes that the ash particles are spherical. We calculate thermal infrared optical properties of highly irregular and porous ash particles and compare these with mass- and volume-equivalent spherical models. Furthermore, brightness temperatures pertinent to satellite observing geometry are calculated for the different ash particle shapes. Non-spherical shapes and volume-equivalent spheres are found to produce a detectable ash signal for larger particle sizes than mass-equivalent spheres. The assumption of mass-equivalent spheres for ash mass loading estimates will underestimate the mass loading by several tens of percent compared to morphologically complex inhomogeneous ash particles.

Description: Role of coarse and fine mode aerosols in MODIS AOD retrieval: a case study Atmospheric Measurement Techniques Discussions, 6, 9109-9132, 2013 Author(s): M. N. Sai Suman, H. Gadhavi, V. Ravi Kiran, A. Jayaraman, and S. V. B. Rao In the present study we have compared the MODIS (Moderate Resolution Imaging Spectroradiometer) derived aerosol optical depth (AOD) data with that obtained from operating sky-radiometer at a remote rural location in South India (Gadanki, 13.45° N, 79.18° E). While the comparison between total (coarse mode + fine mode) AOD shows R 2 value of about 0.71 with a negligible bias of 0.01, if one separates the AOD into fine and coarse mode, the comparison becomes very poor, particularly for fine mode with an R 2 value of 0.44. The coarse mode AOD derived from MODIS and sky-radiometer compare better with an R 2 value of 0.74 and also the seasonal variation is well captured by both measurements. It is shown that the fine mode fraction derived from MODIS data is more than a factor of two smaller than that derived from the sky-radiometer data. Based on these observations we argue that the selection of aerosol types used in the MODIS retrieval algorithm are not appropriate particularly in the case of South India. Instead of selecting a moderately absorbing aerosol type (as being done currently in the MODIS retrieval) a more absorbing type aerosol is better suited for fine mode aerosols, while reverse is true for the coarse mode aerosols, where instead of using "dust aerosols" which is relatively more absorbing, usage of coarse sea-salt particles which is less absorbing is more appropriate.

Description: Freezing nucleation apparatus puts new slant on study of biological ice nucleators in precipitation Atmospheric Measurement Techniques Discussions, 6, 9163-9180, 2013 Author(s): E. Stopelli, F. Conen, L. Zimmermann, C. Alewell, and C. E. Morris Since decades, drop-freezing instruments have contributed to a better understanding of biological ice nucleation and its likely implications on cloud and precipitation development. Yet, current instruments have limitations. Drops analysed on a cold stage are subject to evaporation and potential contamination. The use of closed tubes provides a partial solution to these problems, but freezing events are still difficult to be clearly detected. Here, we present a new apparatus where freezing in closed tubes is detected automatically by a change in light transmission upon ice development, caused by the formation of air bubbles and crystal facets that scatter light. Risks of contamination and introduction of biases linked to detecting the freezing temperature of a sample are then minimized. To illustrate the performance of the new apparatus we show initial results of two assays with snow samples. In one, we repeatedly analysed the sample (208 tubes) over the course of a month with storage at +4 °C, during which evidence for biological ice nucleation activity emerged through an increase in the number of ice nucleators active around −4 °C. In the second assay, we indicate the possibility to increasingly isolate a single ice nucleator from a precipitation sample, potentially determining the nature of a particle responsible for a nucleation activity measured directly in the sample. These two seminal approaches highlight the relevance of this handy apparatus to provide new points of view in biological ice nucleation research.

Description: Unconstrained, robust Kalman filtering for GNSS troposphere tomography Atmospheric Measurement Techniques Discussions, 6, 9133-9162, 2013 Author(s): W. Rohm, K. Zhang, and J. Bosy The mesoscale variability of water vapour (WV) in the troposphere is a highly complex phenomenon and modeling and monitoring the WV distribution is a very important but challenging task. Any observation technique that can reliably provide WV distribution is essential for both monitoring and predicting weather. GNSS tomography technique is a powerful tool that builds upon the critical ground-based GNSS infrastructure – Continuous Operating Reference Station (CORS) networks and can be used to sense the amount of WV. Previous research suggests that 3-D WV field from GNSS tomography has an uncertainty of 1 hPa. However all the models used in GNSS tomography heavily rely on a priori information and constraints from non-GNSS measurements. In this study, 3-D GNSS tomography models are investigated based on an unconstrained approach with limited a priori information. A case study is designed and the results show that unconstrained solutions are feasible by using a robust Kalman filtering technique and effective removal of linearly dependent observations and parameters. Discrepancies between reference wet refractivity data derived from the Australian Numerical Weather Prediction (NWP) model (i.e. ACCESS) and the GNSS tomography model using both simulated and real data are 4.2 ppm (mm km −1 ) and 6.5 ppm (mm km −1 ), respectively, which are essentially in the same order of accuracy. Therefore the accuracy of the integrated values should not be worse than 0.06 m in terms of zenith wet delay and the integrated water vapour is a fifth of this value which is roughly 10 mm.

Description: Vertical profile of δ 18 OOO from middle stratosphere to lower mesosphere derived by retrieval algorithm developed for SMILES spectra Atmospheric Measurement Techniques Discussions, 6, 8889-8935, 2013 Author(s): T. O. Sato, H. Sagawa, N. Yoshida, and Y. Kasai Ozone is known to have large oxygen isotopic enrichments of about 10 % in the middle stratosphere, however, there have been no reports on ozone isotopic enrichments above the middle stratosphere. We derived an enrichment δ 18 OOO by a retrieval algorithm specified for the isotopic ratio from the stratosphere to the lower mesosphere based on observations from the Superconducting Submillimeter-Wave Limb–Emission Sounder (SMILES) onboard the International Space Station (ISS). The retrieval algorithm includes (i) an a priori covariance matrix constrained by oxygen isotopic ratios in ozone, (ii) an optimization of spectral windows for ozone isotopomers and isotopologues, and (iii) a common tangent height information for all windows. The δ 18 OOO obtained by averaging the SMILES measurements at the latitude range of 20° N to 40° N from February to March in 2010 with solar zenith angle

Description: Retrieving aerosol height from the oxygen A band: a fast forward operator and sensitivity study concerning spectral resolution, instrumental noise, and surface inhomogeneity Atmospheric Measurement Techniques Discussions, 6, 10511-10550, 2013 Author(s): A. Hollstein and J. Fischer Hyperspectral radiance measurements in the oxygen A band are sensitive to the vertical distribution of atmospheric scatterers, which in principle allows to retrieve aerosol height from future instruments like TROPOMI, OCO2, FLEX, and CarbonSat. Discussed in this paper is a fast and flexible forward operator for the simulation of hyperspectral radiances in the oxygen A band and, based on this scheme, a sensitivity study about the inversion quality of aerosol optical thickness, aerosol mean height, and aerosol type. The forward operator is based on a lookup table with efficient data compression based on principal component analysis. Linear interpolation and computation of partial derivatives is performed in the much smaller space of expansion coefficients rather then wavelength. Thus, this approach is computationally fast and at the same time memory efficient. The sensitivity study explores the impact of instrument design on the retrieval of aerosol optical thickness and aerosol height. Considered are signal to noise ratio, spectral resolution, and spectral sampling. Also taken into account are surface inhomogeneities and variations of the aerosol type.

Description: The large-scale spatio-temporal variability of precipitation over Sweden observed from the weather radar network Atmospheric Measurement Techniques Discussions, 6, 10699-10730, 2013 Author(s): A. Devasthale and L. Norin Using measurements from the national network of 12 weather radar stations for the last decade (2000–2010), we investigate the large-scale spatio-temporal variability of precipitation over Sweden. These statistics provide useful information to evaluate regional climate models as well as for hydrology and energy applications. A strict quality control is applied to filter out noise and artifacts from the radar data. We focus on investigating four distinct aspects namely, the diurnal cycle of precipitation and its seasonality, the dominant time scale (diurnal vs. seasonal) of variability, precipitation response to different wind directions, and the correlation of precipitation events with the North Atlantic Oscillation (NAO) and the Arctic Oscillation (AO). When classified based on their intensity, moderate to high intensity events (precipitation 〉 0.34 mm (3 h) −1 ) peak distinctly during late afternoon over the majority of radar stations in summer and during late night or early morning in winter. Precipitation variability is highest over the southwestern parts of Sweden. It is shown that the high intensity events (precipitation 〉 1.7mm (3 h) −1 ) are positively correlated with NAO and AO (esp. over northern Sweden), while the low intensity events are negatively correlated (esp. over southeastern parts). It is further observed that southeasterly winds often lead to intense precipitation events over central and northern Sweden, while southwesterly winds contribute most to the total accumulated precipitation for all radar stations. Apart from its operational applications, the present study demonstrates the potential of the weather radar data set for studying climatic features of precipitation over Sweden.

Description: The response of super pressure balloons to gravity wave motions Atmospheric Measurement Techniques Discussions, 6, 10797-10832, 2013 Author(s): R. A. Vincent and A. Hertzog Super pressure balloons (SPB), which float on constant density (isopycnic) surfaces, provide a unique way of measuring the properties of atmospheric gravity waves (GW) as a function of wave intrinsic frequency. Here we devise a quasi-analytic method of investigating the SPB response to GW motions. It is shown that the results agree well with more rigorous numerical simulations of balloon motions and provide a better understanding of the response of SPB to GW, especially at high frequencies. The methodology is applied to ascertain the accuracy of GW studies using 12 m diameter SPB deployed in the 2010 Concordiasi campaign in the Antarctic. In comparison with the situation in earlier campaigns, the vertical displacements of the SPB were measured directly using GPS. It is shown using a large number of Monte-Carlo type simulations with realistic instrumental noise that important wave parameters, such as momentum flux, phase speed and wavelengths, can be retrieved with good accuracy from SPB observations for intrinsic wave periods greater than about 10 min. The noise floor for momentum flux is estimated to be about 10 −4 mPa.

Description: Inversion of droplet aerosol analyzer data for long-term aerosol-cloud interaction measurements Atmospheric Measurement Techniques Discussions, 6, 10269-10295, 2013 Author(s): M. I. A. Berghof, G. P. Frank, S. Sjogren, and B. G. Martinsson The droplet aerosol analyzer (DAA) was developed to study the influence of aerosol properties on clouds. It measures the ambient particle size of individual droplets and interstitial particles, the size of the dry (residual) particles after the evaporation of water, and the number concentration of the dry (residual) particles. A method was developed for the evaluation of DAA data to obtain the three-parameter dataset: ambient particle diameter, dry (residual) particle diameter and number concentration. First results from in-cloud measurements performed on the summit of Mt. Brocken in Germany are presented. Various aspects of the cloud aerosol dataset are presented, such as the number concentration of interstitial particles and cloud droplets, the dry residue particle size distribution, droplet size distributions, scavenging ratios due to cloud droplet formation and size-dependent solute concentrations. This dataset makes it possible to study clouds and the influence of the aerosol population on clouds.

Description: Calibrated high-precision 17 O excess measurements using laser-current tuned cavity ring-down spectroscopy Atmospheric Measurement Techniques Discussions, 6, 10191-10229, 2013 Author(s): E. J. Steig, V. Gkinis, A. J. Schauer, S. W. Schoenemann, K. Samek, J. Hoffnagle, K. J. Dennis, and S. M. Tan High precision analysis of the 17 O/ 16 O isotope ratio in water and water vapor is of interest in hydrological, paleoclimate, and atmospheric science applications. Of specific interest is the parameter 17 O excess , a measure of the deviation from a linear relationship between 17 O/ 16 O and 18 O/ 16 O ratios. Conventional analyses of 17 O excess are obtained by fluorination of H 2 O to O 2 that is analyzed by dual-inlet isotope ratio mass spectrometry (IRMS). We describe a new laser spectroscopy instrument for high-precision 17 O excess measurements. The new instrument uses cavity ring-down spectroscopy (CRDS) with laser-current tuning to achieve reduced measurement drift compared with previous-generation instruments. Liquid water and water vapor samples can be analyzed with better than 8 per meg precision for 17 O excess using integration times of less than 30 min. Calibration with respect to accepted water standards demonstrates that both the precision and the accuracy are competitive with conventional IRMS methods. The new instrument also achieves simultaneous measurements of δ 18 O, 17 Oand δD with precision 〈 0.03‰, 〈 0.02‰ and 〈 0.2‰, respectively.

Description: Clues for a standardised thermal-optical protocol for the assessment of organic and elemental carbon within ambient air particulate matter Atmospheric Measurement Techniques Discussions, 6, 10231-10268, 2013 Author(s): L. Chiappini, S. Verlhac, R. Aujay, W. Maenhaut, J. P. Putaud, J. Sciare, J. L. Jaffrezo, C. Liousse, C. Gally-Lacaux, L. Alleman, P. Panteliadis, E. Leoz, and O. Favez Along with some research networking programs, the European Directive 2008/50/CE requires chemical speciation of fine aerosol (PM 2.5 ), including elemental (EC) and organic carbon (OC), at a few rural sites in European countries. Meanwhile, the thermal-optical technique is considered by the European and US networking agencies and normalization bodies as a reference method to quantify EC–OC collected on filters. Although commonly used for many years, this technique is still suffering from a lack of information on the comparability of the different analytical protocols (temperature protocols, type of optical correction) currently applied in the laboratories. To better evaluate the EC–OC data set quality and related uncertainties, the French National Reference Laboratory for Ambient Air Quality Monitoring (LCSQA) has organized an EC–OC comparison exercise for French laboratories using different thermal-optical methods. While there is good agreement on total carbon (TC) measurements among all participants, some discrepancies can be observed on the EC/TC ratio, even among laboratories using the same thermal protocol. These results led to further tests on the influence of the optical correction: results obtained from different European Laboratories, confirming that there are higher differences between OC TOT and OC TOR measured with NIOSH 5040 in comparison to EUSAAR-2. Also, striking differences between EC TOT /EC TOT ratios can be observed when comparing rural and urban results whatever the thermal protocol EC TOT being 50% lower than EC TOT at rural sites whereas it is only 20% lower at urban sites. The PM chemical composition could explain these differences but the way it influences the EC–OC measurement is not clear and needs further investigations. Meanwhile, some additional tests seem to indicate an influence of the oven soiling on the EC–OC measurement data quality. This enlightens the necessity to follow the laser signal decrease with time and its impact on measurements. Nevertheless, this should be confirmed by further experiments, involving more samples and various instruments, to enable statistical processing. All these results provide insights to determine the quality of EC–OC analytical methods and may contribute to the work toward establishing method standardisation.

Description: A video precipitation sensor for imaging and velocimetry of hydrometeors Atmospheric Measurement Techniques Discussions, 6, 10165-10189, 2013 Author(s): X. C. Liu, T. C. Gao, and L. Liu A new method to determine the shape and fall velocity of hydrometeors by using a single CCD camera is proposed in this paper, and a prototype of Video Precipitation Sensor (VPS) is developed. The instrument consists of an optical unit (collimated light source with multi-mode fiber cluster), an imaging unit (planar array CCD sensor), an acquisition and control unit, and a data processing unit, the cylindrical space between the optical unit and imaging unit is sampling volume (300 mm × 40 mm × 30 mm). As the precipitation particles fall through the sampling volume, the CCD camera exposures two times in a single frame, by which the double-exposure of particles images can be obtained. The size and shape can be obtained by the images of particles; the fall velocity can be calculated by particle displacement in double-exposure image and interval time; the drop size distribution and velocity distribution, precipitation intensity, and accumulated precipitation amount can be calculated by time integration. The innovation of VPS is that the shape, size, and velocity of precipitation particles can be measured by only one planar array CCD sensor, which can address the disadvantages of linear scan CCD disdrometer and impact disdrometer. Field measurements of rainfall demonstrate the VPS's capability to measure micro-physical properties of single particles and integral parameters of precipitation.

Description: Comparison of profile total ozone from SBUV(v8.6) with GOME-type and ground-based total ozone for 16-yr period (1996 to 2011) Atmospheric Measurement Techniques Discussions, 6, 10081-10115, 2013 Author(s): E. W. Chiou, P. K. Bhartia, R. D. McPeters, D. G. Loyola, M. Coldewey-Egbers, V. E. Fioletov, M. Van Roozendael, C. Lerot, R. Spurr, and S. M. Frith This paper describes the comparison of the variability of total column ozone inferred from the three independent multi-year data records, namely, (i) SBUV(v8.6) profile total ozone, (ii) GTO(GOME-Type total ozone), and (iii) Ground-based total ozone data records covering the 16-yr overlap period (March 1996 through June 2011). Analyses are conducted based on area weighted zonal means for (0–30° S), (0–30° N), (50–30° S), and (30–60° N). It has been found that on average, the differences in monthly zonal mean total ozone vary between −0.32 to 0.76 % and are well within 1%. For "GTO minus SBUV", the standard deviations and ranges (maximum minus minimum) of the differences regarding monthly zonal mean total ozone vary between 0.58 to 0.66% and 2.83 to 3.82% respectively, depending on the latitude band. The corresponding standard deviations and ranges regarding the differences in monthly zonal mean anomalies show values between 0.40 to 0.59% and 2.19 to 3.53%. The standard deviations and ranges of the differences "Ground-based minus SBUV" regarding both monthly zonal means and anomalies are larger by a factor of 1.4 to 2.9 in comparison to "GTO minus SBUV". The Ground-based zonal means, while show no systematic differences, demonstrate larger scattering of monthly data compared to satellite-based records. The differences in the scattering are significantly reduced if seasonal zonal averages are analyzed. The trends of the differences "GTO minus SBUV" and "Ground-based minus SBUV" are found to vary between −0.04 and 0.12% yr −1 (−0.11 and 0.31 DU yr −1 ). These negligibly small trends have provided strong evidence that there are no significant time dependent differences among these multi-year total ozone data records. Analyses of the deviations from pre-1980 level indicate that for the overlap period of 1996 to 2010, all three data records show gradual recovery at (30–60° N) from −5% in 1996 to −2% in 2010. The corresponding recovery at (50–30° S) is not as obvious until after 2006.

Description: Open-path, quantum cascade laser-based sensor for high resolution atmospheric ammonia measurements Atmospheric Measurement Techniques Discussions, 6, 7005-7039, 2013 Author(s): D. J. Miller, K. Sun, L. Tao, M. A. Khan, and M. A. Zondlo We demonstrate a compact, open-path, quantum cascade laser-based atmospheric ammonia sensor operating at 9.06 μm for high sensitivity, high temporal resolution, ground-based measurements. Atmospheric ammonia (NH 3 ) is a gas-phase precursor to fine particulate matter, with implications for air quality and climate change. Currently, NH 3 sensing challenges have led to a lack of widespread in-situ measurements. Our open-path sensor configuration avoids sampling artifacts associated with NH 3 surface adsorption onto inlet tubing and reduced pressure sampling cells, as well as condensed-phase partitioning ambiguities. Multi-harmonic wavelength modulation spectroscopy allows for selective and sensitive detection of atmospheric-pressure broadened absorption features. An in-line ethylene reference cell provides real-time calibration (±20% accuracy) and normalization for instrument drift under rapidly changing field conditions. The sensor has a sensitivity and minimum detection limit of 0.15 ppbv NH 3 at 10 Hz, a mass of ~ 5 kg and consumes ~ 50 W of electrical power. In-situ field performance of this open-path NH 3 sensor is demonstrated, with 10 Hz time resolution and a large dynamic response for in-situ NH 3 measurements. This sensor provides the capabilities for improved in-situ gas phase NH 3 sensing relevant for emission source characterization and flux measurements.

Description: Trajectory matching of ozonesondes and MOZAIC measurements in the UTLS – Part 1: Method description and application at Payerne, Switzerland Atmospheric Measurement Techniques Discussions, 6, 7063-7098, 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 ozone 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

Description: Vertical air motions derived from a descending radiosonde using a lightweight hard ball as the parachute Atmospheric Measurement Techniques Discussions, 6, 8107-8127, 2013 Author(s): H. Chen, Y. Zhu, J. Zhang, and Y. Xuan Knowledge of vertical air motions in the atmosphere is important for meteorological and climate studies due to its impact on clouds, precipitation and the vertical transport of air masses, heat, momentum, and composition. It is among the most difficult quantities to measure because of its small magnitude. In this study, a descending radiosonde technique has been developed to detect the vertical wind speed (VW) in the atmosphere. The system is composed of a radiosonde and a 0.5-m diameter hard ball made of plastic foam that acts as a parachute. The radiosonde hangs under the hard ball by a string which is then cut when the instrument is elevated into the upper troposphere by a balloon. The VW is derived from the difference between the observed radiosonde descent rate and the calculated radiosonde descent rate in still air based on fluid dynamics. Deduction of the appropriate drag coefficient for the radiosonde is facilitated by the symmetrical shape of the parachute. An intensive radiosonde launch experiment was held in northern China during the summer seasons of 2010 to 2012. This study uses radiosonde data collected during the campaign to retrieve the vertical air velocity within the radiosonde altitude-detecting range. In general, the VW ranges from −1 to 1 m s −1 . Strong vertical air motion (~2 m s −1 ) is seen in a few radiosonde measurements. Although considerable uncertainties exist in measuring weak vertical air motions, a case study shows that there is reasonable agreement between retrievals of VW in the lower atmosphere from the radiosonde and a wind profiler radar located at the launch site.

Description: Long-path averaged mixing ratios of O 3 and NO 2 in the free troposphere from mountain MAX-DOAS Atmospheric Measurement Techniques Discussions, 6, 8235-8267, 2013 Author(s): L. Gomez, M. Navarro-Comas, O. Puentedura, Y. Gonzalez, E. Cuevas, and M. Gil-Ojeda A new approximation is proposed to estimate O 3 and NO 2 mixing ratios in the Northern Subtropics Free Troposphere (FT). Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) high mountain measurements, recorded at Izaña Observatory (28°18' N, 16°29' W), are used in this work. Proposed method uses horizontal and near-zenith geometries to estimate the station level differential path. Two different methods are described. First one uses retrieved Slant Column Densities (SCD) of O 4 . On second method, path is estimated from LIBRADTRAN radiative transfer model for the region and season. Results show that under low aerosol loading, O 3 and NO 2 mixing ratios concentrations can be retrieved with moderately low errors. Obtained concentrations have been compared with in situ instrumentation on the observatory. O 3 concentration in FT is found to be in the range of 40–80 ppb, approximately. NO 2 is in the range of 20–30 ppt, below the detection limit of in situ instrumentation. The different air masses scanned by each instrument have been identified as a cause of discrepancy between O 3 observed by MAX-DOAS and in situ.

Description: A feasibility study for the retrieval of the total column precipitable water vapor from satellite observations in the blue spectral range Atmospheric Measurement Techniques Discussions, 6, 3643-3674, 2013 Author(s): T. Wagner, S. Beirle, H. Sihler, and K. Mies We present a new algorithm for satellite retrievals of the atmospheric water vapor column in the blue spectral range. The water vapor 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 is systematically larger than for retrievals at longer wavelengths. Nevertheless, water vapor 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 vapor retrievals are more consistent than for longer wavelengths. Compared to retrievals at longer wavelengths, over ocean 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 vapor 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 vapor 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 vapor 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 like e.g. Sentinel 4 and 5.

Description: Implementation of a 3-D-Var system for atmospheric profiling data assimilation into the RAMS model: initial results Atmospheric Measurement Techniques Discussions, 6, 3581-3610, 2013 Author(s): S. Federico This paper presents the current status of development of a three-dimensional variational data assimilation system. The system can be used with different numerical weather prediction models, but it is mainly designed to be coupled with the Regional Atmospheric Modelling System (RAMS). Analyses are given for the following parameters: zonal and meridional wind components, temperature, relative humidity, and geopotential height. Important features of the data assimilation system are the use of incremental formulation of the cost-function, and the use of an analysis space represented by recursive filters and eigenmodes of the vertical background error matrix. This matrix and the length-scale of the recursive filters are estimated by the National Meteorological Center (NMC) method. The data assimilation and forecasting system is applied to the real context of atmospheric profiling data assimilation, and in particular to the short-term wind prediction. The analyses are produced at 20 km horizontal resolution over central Europe and extend over the whole troposphere. Assimilated data are vertical soundings of wind, temperature, and relative humidity from radiosondes, and wind measurements of the European wind profiler network. Results show the validity of the analysis solutions because they are closer to the observations (lower RMSE) compared to the background (higher RMSE), and the differences of the RMSEs are consistent with the data assimilation settings. To quantify the impact of improved initial conditions on the short-term forecast, the analyses are used as initial conditions of a three-hours forecast of the RAMS model. In particular two sets of forecasts are produced: (a) the first uses the ECMWF analysis/forecast cycle as initial and boundary conditions; (b) the second uses the analyses produced by the 3-D-Var scheme as initial conditions, then is driven by the ECMWF forecast. The improvement is quantified by considering the horizontal components of the wind, which are measured at a-synoptic times by the European wind profiler network. The results show that the RMSE is effectively reduced at the short range (1–2 h). The results are in agreement with the set-up of the numerical experiment.

Description: Tropospheric CO vertical profiles deduced from total columns using data assimilation: methodology and validation Atmospheric Measurement Techniques Discussions, 6, 6517-6566, 2013 Author(s): L. El Amraoui, J.-L. Attié, P. Ricaud, W. A. Lahoz, A. Piacentini, V.-H. Peuch, J. X. Warner, R. Abida, and J. Barré This paper presents a validation of a method to derive the vertical profile of carbon monoxide (CO) from its total column using data assimilation. The main motivation of this study is twofold. First, to deduce both the vertical CO profiles and the assimilated CO fields with good confidence. Second, for chemical species that can be measured only as the total column, this method provides an attractive alternative for estimating their vertical profiles in the troposphere. We choose version 3 (V3) of MOPITT CO total columns to validate the proposed method. MOPITT has the advantage of providing both the vertical profiles and the total columns of CO. Furthermore, this version has been extensively validated by comparison with many independent datasets, and has been used in many scientific studies. The first step of the paper consists in the specification of the observation errors based on the Chi-square (χ 2 ) test. The observations have been binned according to day, night, land and sea (LAND_DAY, LAND_NIGHT and SEA, respectively). The respective optimal observation error values for which the χ 2 metric is the closest to 1 are: 7%, 8% and 11% for SEA, LAND_DAY and LAND_NIGHT, respectively. In a second step, the CO total column, with its specified errors, is used within the assimilation system to estimate the vertical profiles. These are validated by comparison with vertical profiles of MOPITT V3 retrievals at global and regional scales. Generally, both datasets show similar patterns and good agreement at both global and regional scales. Nevertheless, the total column analyses (TOTCOL_ANALYSES) slightly overestimate CO concentrations compared to MOPITT observations. In a third step, vertical profiles calculated from TOTCOL_ANALYSES have been compared to those calculated from the assimilation of MOPITT V3 vertical profiles (PROFILE_ANALYSES). Both datasets shows very good agreement, but TOTCOL_ANALYSES tend to slightly overestimate CO concentrations. The mean bias between both datasets is 6% and 8% at the pressure levels 700 and 200 hPa, respectively. In terms of zonal means, the CO distribution is similar for both analyses. The mean bias between these datasets is low and doesn't exceed 12%. These results confirm that both analyses (total column and vertical profiles) are in very good agreement at global and regional scales.

Description: HCl and ClO profiles inside the Antarctic vortex as observed by SMILES in November 2009: comparisons with MLS and ACE-FTS instruments Atmospheric Measurement Techniques Discussions, 6, 6729-6765, 2013 Author(s): T. Sugita, Y. Kasai, Y. Terao, S. Hayashida, G. L. Manney, W. H. Daffer, H. Sagawa, M. Suzuki, M. Shiotani, K. A. Walker, C. D. Boone, and P. F. Bernath We present vertical profiles of hydrogen chloride (HCl) and chlorine monoxide (ClO) as observed by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) inside the Antarctic vortex on 19–24 November 2009. The SMILES HCl value reveals 2.8–3.1 ppbv between 450 and 500 K levels in potential temperature (PT). The high value of HCl is highlighted since it is suggested that HCl was a main component of the total inorganic chlorine (Cly), defined as Cly ≃ HCl + ClO + chlorine nitrate (ClONO 2 ) inside the Antarctic vortex in spring, owing to low ozone values. To confirm the quality of two SMILES Level 2 (L2) data products provided by Japan Aerospace Exploration Agency (JAXA) and National Institute of Information and Communications Technology (NICT) from a view point of the partitioning of Cly, comparisons are made using other satellite data, from the Aura Microwave Limb Sounder (MLS) and Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS). HCl values from the SMILES NICT L2 product agree to within 10% with the MLS HCl data between 425 and 650 K levels in PT and with the ACE-FTS HCl data between 425 and 575 K, respectively. The SMILES JAXA L2 product is 10 to 20% smaller than that from MLS (ACE-FTS) between 400 (500 K) and 700 K. For ClO in daytime, the difference between SMILES (JAXA and NICT) and MLS was less than ±0.05 ppbv between 500 and 650 K with the ClO values less than 0.2 ppbv. ClONO 2 values as measured by ACE-FTS also reveal 0.2 ppbv at 475–500 K level, resulting in the HCl/Cly ratios of 0.91–0.95. The high HCl value and HCl/Cly ratio found from the three satellite instruments agree with the past observations inside the Antarctic vortex at this time (October to November) of year in the lower stratosphere.

Description: Light extinction by Secondary Organic Aerosol: an intercomparison of three broadband cavity spectrometers Atmospheric Measurement Techniques Discussions, 6, 6685-6727, 2013 Author(s): R. M. Varma, S. M. Ball, T. Brauers, H.-P. Dorn, U. Heitmann, R. L. Jones, U. Platt, D. Pöhler, A. A. Ruth, A. J. L. Shillings, J. Thieser, A. Wahner, and D. S. Venables Broadband optical cavity spectrometers are maturing as a technology for trace gas detection, but only recently have they been used to retrieve the extinction coefficient of aerosols. Sensitive broadband extinction measurements allow explicit separation of gas and particle phase spectral contributions, as well as continuous spectral measurements of aerosol extinction in favourable cases. In this work, we report an intercomparison study of the aerosol extinction coefficients measured by three such instruments: a broadband cavity ring-down spectrometer (BBCRDS), a cavity-enhanced differential optical absorption spectrometer (CE-DOAS), and an incoherent broadband cavity-enhanced absorption spectrometer (IBBCEAS). Experiments were carried out in the SAPHIR atmospheric simulation chamber as part of the NO3Comp campaign to compare the measurement capabilities of NO 3 and N 2 O 5 instrumentation. Aerosol extinction coefficients between 655 and 690 nm are reported for secondary organic aerosols (SOA) formed by the NO 3 oxidation of β-pinene under dry and humid conditions. Despite different measurement approaches and spectral analysis procedures, the three instruments retrieved aerosol extinction coefficients that were in close agreement. The refractive index of SOA formed from the β-pinene + NO 3 reaction was 1.61, and was not measurably affected by the chamber humidity or by aging of the aerosol over several hours. This refractive index is significantly larger than SOA refractive indices observed in other studies of OH and ozone-initiated terpene oxidations, and may be caused by the large proportion of organic nitrates in the particle phase. In an experiment involving ammonium sulphate particles the aerosol extinction coefficients as measured by IBBCEAS were found to be in reasonable agreement with those calculated using Mie theory. The results of the study demonstrate the potential of broadband cavity spectrometers for determining the optical properties of aerosols.

Description: Space-based retrieval of NO 2 over biomass burning regions: quantifying and reducing uncertainties Atmospheric Measurement Techniques Discussions, 6, 6645-6684, 2013 Author(s): N. Bousserez The quality of space-based nitrogen dioxide (NO 2 ) retrievals from solar backscatter depends on a priori knowledge of the vertical profiles of NO 2 and aerosol optical properties. This information is contained in an air mass factor (AMF), which accounts for atmospheric scattering and is used to convert the measured line-of-sight "slant" columns into vertical columns. In this study we investigate the impact of biomass burning emissions on the AMF in order to quantify NO 2 retrieval errors in the Ozone Monitoring Instrument (OMI) products over these sources. Sensitivity analyses are conducted using the Linearized Discrete Ordinate Radiative Transfer (LIDORT) model and the GEOS-Chem chemistry-transport model with an improved daily biomass burning emission inventory. Aircraft in situ data collected during two field campaigns, Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) and Dust and Biomass-burning Experiment (DABEX), are used to evaluate the modeled aerosol optical properties and NO 2 profiles over Canadian boreal fires and western Africa savanna fires respectively. Biomass burning aerosols increase the AMF by 3 to 15% over boreal fires, while they decrease the AMF by −10 to −30% over savanna fires. The presence of an elevated aerosol layer over west Africa due to the Harmattan front explains the negative aerosol effect over this area. The impact of fires on the AMF is driven by the NO 2 shape profile perturbations, which decrease the AMF by −10 to −60% over both regions. Aerosol and shape factor effects are most sensitive to surface reflectance and clouds. In particular, retrieval errors associated with shape factor uncertainties can increase by a factor of 2 due to the presence of clouds. In contrast with conclusions from previous studies, we demonstrate that in the presence of pre-existing clouds, the effect of aerosols on the AMF cannot be fully accounted for through the modified retrieved cloud parameters. Finally, a new method that uses slant column information to correct for shape factor error in the retrieval is proposed and tested over west African fires.

Description: The ToF-ACSM: a portable aerosol chemical speciation monitor with TOFMS detection Atmospheric Measurement Techniques Discussions, 6, 6767-6814, 2013 Author(s): R. Fröhlich, M. J. Cubison, J. G. Slowik, N. Bukowiecki, A. S. H. Prévôt, U. Baltensperger, J. Schneider, J. R. Kimmel, M. Gonin, U. Rohner, D. R. Worsnop, and J. T. Jayne We present a new instrument for monitoring aerosol composition, the economy time-of-flight-aerosol chemical speciation monitor (ToF-ACSM), combining precision of state-of-the-art time-of-flight mass spectrometry with stability, reliability, and easy handling, which are necessities for long-term monitoring operations on the scale of months to years. Based on Aerodyne aerosol mass spectrometer (AMS) technology, the ToF-ACSM provides continuous online measurements of chemical composition and mass of non-refractory submicron aerosol particles. In contrast to the larger AMS, the compact-sized and lower-priced ToF-ACSM does not feature particle sizing, similar to the widely-used quadrupole-ACSM (Q-ACSM). Compared to the Q-ACSM, the ToF-ACSM features a better mass resolution of M /Δ M = 600 and better detection limits on the order of 6 months) on the Jungfraujoch mountain ridge (3580 m a.s.l.) in the Swiss Alps agree quantitatively. Additionally, the mass resolution of the ToF-ACSM is sufficient for basic mass defect resolved peak fitting of the recorded spectra, providing a data stream not accessible to the Q-ACSM. This allows for quantification of certain hydrocarbon and oxygenated fragments (e.g. C 3 H 7 + and C 2 H 3 O + , both occurring at m/Q = 43 Th), as well as improving inorganic/organic separation.

Description: Measuring long chain alkanes in diesel engine exhaust by thermal desorption PTR-MS Atmospheric Measurement Techniques Discussions, 6, 6005-6046, 2013 Author(s): M. H. Erickson, M. Gueneron, and B. T. Jobson A method using thermal desorption sampling and analysis by PTR-MS to measure long chain alkanes (C 12 -C 18 ) and other larger organics associated with diesel engine exhaust emissions is described. Long chain alkanes undergo dissociative proton transfer reactions forming a series of fragment ions with formula C n H 2n+1 . The PTR-MS is insensitive to n-alkanes less than C 8 but displays an increasing sensitivity for larger alkanes. Fragment ion distribution and sensitivity is a function of drift conditions. At 80 Td the most abundant ion fragments from C 10 to C 16 n-alkanes were m/z 57, 71 and 85. The mass spectrum of gasoline and diesel fuel at 80 Td displayed ion group patterns that can be related to known fuel constituents, such as alkanes, alkylbenzenes and cycloalkanes, and other compound groups that are inferred from molecular weight distributions such as dihydronapthalenes and naphthenic monoaromatics. It is shown that thermal desorption sampling of gasoline and diesel engine exhausts at 80 Td allows for discrimination against light alkanes and alkenes which are a major constituent of both exhausts, allowing for quantification of higher molecular weight alkanes from the abundance of C n H 2n+1 fragment ions. Using this approach, the molar abundance of C 12 -C 18 alkanes in diesel engine exhaust was found to be 75% that of the total C 1 -C 4 alkylbenzene abundance. While the PTR-MS mass spectra of gasoline and diesel exhaust looked similar, the abundance of higher molecular weight compounds relative to that of C 4 -alkylbenzenes was much greater in diesel engine exhaust. The abundance patterns of compounds determined by thermal desorption sampling may allow for emission profiles to be developed to better quantify the relative contributions of diesel and gasoline exhaust emissions of larger organic compounds to urban air concentrations.

Description: Photoacoustic and nephelometric spectroscopy of aerosol optical properties with a supercontinuum light source Atmospheric Measurement Techniques Discussions, 6, 6293-6327, 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 were 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: Cloud discrimination in probability density functions of limb scattered sunlight measurements Atmospheric Measurement Techniques Discussions, 6, 6491-6516, 2013 Author(s): E. N. Normand, 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 CALIPSO nadir measurements and to those obtained by Wang et al. (1996) with SAGE II solar occultation measurements.

Description: Intercomparison of stratospheric ozone profiles for the assessment of the upgraded GROMOS radiometer at Bern Atmospheric Measurement Techniques Discussions, 6, 6097-6146, 2013 Author(s): S. Studer, K. Hocke, M. Pastel, S. Godin-Beekmann, and N. Kämpfer Since November 1994, the GROund-based Millimeter-wave Ozone Spectrometer (GROMOS) measures stratospheric and lower mesospheric ozone in Bern, Switzerland (47.95° N, 7.44° E). GROMOS is part of the Network for the Detection of Atmospheric Composition Change (NDACC). In July 2009, a Fast-Fourier-Transform spectrometer (FFTS) has been added as backend to GROMOS. The new FFTS and the original filter bench (FB) measured parallel for over two years. In October 2011, the FB has been turned off and the FFTS is now used to continue the ozone time series. For a consolidated ozone time series in the frame of NDACC, the quality of the stratospheric ozone profiles obtained with the FFTS has to be assessed. The FFTS results from July 2009 to December 2011 are compared to ozone profiles retrieved by the FB. FFTS and FB of the GROMOS microwave radiometer agree within 5% above 20 hPa. A later harmonization of both time series will be realized by taking the FFTS as benchmark for the FB. Ozone profiles from the FFTS are also compared to coinciding lidar measurements from the Observatoire Haute Provence (OHP), France. For the time period studied a maximum mean difference (lidar – GROMOS FFTS) of +3.8% at 3.1 hPa and a minimum mean difference of +1.4% at 8 hPa is found. Further, intercomparisons with ozone profiles from other independent instruments are performed: satellite measurements include MIPAS onboard ENVISAT, SABER onboard TIMED, MLS onboard EOS Aura and ACE-FTS onboard SCISAT-1. Additionally, ozonesondes launched from Payerne, Switzerland, are used in the lower stratosphere. Mean relative differences of GROMOS FFTS and these independent instruments are less than 10% between 50 and 0.1 hPa.

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 Discussions, 6, 6249-6292, 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, 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 longer. For a newly developed RO x LIF cell, used for detection of HO 2 and RO 2 radicals, when running in HO x mode an OH yield of 95% was observed for ethene-derived RO 2 radicals. In experiments in which conditions ensured the conversion of RO 2 to OH was 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 alkane-derived RO 2 radicals, 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 ] + α [RO 2 ] and α 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: Validation of FORMOSAT-3/COSMIC level 2 "atmPrf" global temperature data in the stratosphere Atmospheric Measurement Techniques Discussions, 6, 6187-6213, 2013 Author(s): U. Das and C. J. Pan GPS radio occultations by Formosa Satellite mission-3/Constellation Observing System for Meteorology, Ionosphere, and Climate (FORMOSAT-3/COSMIC) provide refractivity profiles, which are processed real-time to give profiles of temperature and water vapour in the lower atmosphere and electron density in the upper atmosphere. The new "atmPrf" (atmospheric profile) product gives temperature from surface to 0.2 hPa (~60 km). This is a dry temperature data product that does not include relative humidity in the inversion process and hence is reliable at and above the tropopause (〉100 hPa) and erroneous in the troposphere (

Description: Interpretation of observed microwave signatures from ground dual polarization radar and space multi frequency radiometer for the 2011 Grímsvötn volcanic eruption Atmospheric Measurement Techniques Discussions, 6, 6215-6248, 2013 Author(s): M. Montopoli, G. Vulpiani, D. Cimini, E. Picciotti, and F. S. Marzano The important role played by ground-based microwave weather radars for the monitoring of volcanic ash clouds has been recently demonstrated. The potential of microwaves from satellite passive and ground-based active sensors to estimate near-source volcanic ash cloud parameters has been also proposed, though with little investigation of their synergy and the role of the radar polarimetry. The goal of this work is to show the potentiality and drawbacks of the X-band Dual Polarization radar measurements (DPX) through the data acquired during the latest Grímsvötn volcanic eruptions that took place on May 2011 in Iceland. The analysis is enriched by the comparison between DPX data and the observations from the satellite Special Sensor Microwave Imager/Sounder (SSMIS) and a C-band Single Polarization (SPC) radar. SPC, DPX, and SSMIS instruments cover a large range of the microwaves spectrum, operating respectively at 5.4, 3.2, and 0.16–1.6 cm wavelengths. The multi-source comparison is made in terms of Total Columnar Concentration (TCC). The latter is estimated from radar observables using the "Volcanic Ash Radar Retrieval for dual-Polarization X band systems" (VARR-PX) algorithm and from SSMIS brightness temperature (BT) using a linear BT–TCC relationship. The BT–TCC relationship has been compared with the analogous relation derived from SSMIS and SPC radar data for the same case study. Differences between these two linear regression curves are mainly attributed to an incomplete observation of the vertical extension of the ash cloud, a coarser spatial resolution and a more pronounced non-uniform beam filling effect of SPC measurements (260 km far from the volcanic vent) with respect to the DPX (70 km from the volcanic vent). Results show that high-spatial-resolution DPX radar data identify an evident volcanic plume signature, even though the interpretation of the polarimetric variables and the related retrievals is not always straightforward, likely due to the possible formation of ash and ice particle aggregates and the radar signal depolarization induced by turbulence effects. The correlation of the estimated TCCs derived from DPX and SSMIS BTs reaches −0.73.

Description: Characterization of disdrometer uncertainties and impacts on estimates of snowfall rate and radar reflectivity Atmospheric Measurement Techniques Discussions, 6, 6329-6369, 2013 Author(s): N. B. Wood, T. S. L'Ecuyer, F. L. Bliven, and G. L. Stephens Estimates of snow microphysical properties obtained by analyzing collections of individual particles are often limited to short time scales and coarse time resolution. Retrievals using disdrometer observations coincident with bulk measurements such as radar reflectivity and snowfall amounts may overcome these limitations; however, retrieval techniques using such observations require uncertainty estimates not only for the bulk measurements themselves, but also for the simulated measurements modeled from the disdrometer observations. Disdrometer uncertainties arise due to sampling and analytic errors and to the discrete, potentially truncated form of the reported size distributions. Imaging disdrometers such as the Snowflake Video Imager and 2-D Video Disdrometer provide remarkably detailed representations of snow particles, but view limited projections of their three-dimensional shapes. Particle sizes determined by such instruments underestimate the true dimensions of the particles in a way that depends, in the mean, on particle shape, also contributing to uncertainties. An uncertainty model that accounts for these uncertainties is developed and used to establish their contributions to simulated radar reflectivity and snowfall rate. Viewing geometry effects are characterized by a parameter, φ, that relates disdrometer-observed particle size to the true maximum dimension of the particle. Values and uncertainties for φ are estimated using idealized ellipsoidal snow particles. The model is applied to observations from seven snow events from the Canadian CloudSat CALIPSO Validation Project (C3VP), a mid-latitude cold season cloud and precipitation field experiment. Typical total uncertainties are 4 dBZ for reflectivity and 40–60% for snowfall rate, are highly correlated, and are substantial compared to expected observational uncertainties. The dominant sources of errors are viewing geometry effects and the discrete, truncated form of the size distributions. While modeled Ze- S relationships are strongly affected by assumptions about snow particle mass properties, such relationships are only modestly sensitive to φ owing to partially compensating effects on both the reflectivity and snowfall rate.

Description: SoFi, an Igor based interface for the efficient use of the generalized multilinear engine (ME-2) for source apportionment: application to aerosol mass spectrometer data Atmospheric Measurement Techniques Discussions, 6, 6409-6443, 2013 Author(s): F. Canonaco, M. Crippa, J. G. Slowik, U. Baltensperger, and A. S. H. Prévôt Source apportionment using the bilinear model through the multilinear engine (ME-2) was successfully applied to non-refractory organic aerosol (OA) mass spectra collected during winter 2011 and 2012 in Zurich, Switzerland using the aerosol chemical speciation monitor ACSM. Five factors were identified: low-volatility oxygenated OA (LV-OOA), semivolatile oxygenated OA (SV-OOA), hydrocarbon-like OA (HOA), cooking OA (COA) and biomass burning OA (BBOA). A graphical user interface SoFi (Source Finder) was developed at PSI in order to facilitate the testing of different rotational techniques available within the ME-2 engine by providing a priori factor profiles for some or all of the expected factors. ME-2 was used to test the positive matrix factorization (PMF) model, the fully constrained chemical mass balance (CMB) model, and partially constrained models utilizing a values and pulling equations. Within the set of model solutions determined to be environmentally reasonable, BBOA and SV-OOA factor mass spectra and time series showed the greatest variability. This variability represents uncertainty in the model solution and indicates that analysis of model rotations provides a useful approach for assessing the uncertainty of bilinear source apportionment models.

Description: Characterization of an aerodynamic lens for transmitting particles 〉 1 micrometer in diameter into the Aerodyne aerosol mass spectrometer Atmospheric Measurement Techniques Discussions, 6, 5033-5063, 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 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: A global climatology of stratospheric OClO derived from GOMOS measurement Atmospheric Measurement Techniques Discussions, 6, 3511-3543, 2013 Author(s): C. Tétard, D. Fussen, F. Vanhellemont, C. Bingen, E. Dekemper, N. Mateshvili, D. Pieroux, C. Robert, E. Kyrölä, J. Tamminen, V. Sofieva, A. Hauchecorne, F. Dalaudier, J.-L. Bertaux, O. Fanton d'Andon, G. Barrot, L. Blanot, A. Dehn, and L. Saavedra de Miguel The Global Ozone Monitoring by Occultation of Stars (GOMOS) instrument on board the European platform ENVISAT was dedicated to the study of the atmosphere of the Earth using the stellar occultation technique. The spectral range of the GOMOS spectrometer extends from the UV to the near infrared, allowing for the retrieval of species such as O 3 , NO 2 , NO 3 , H 2 O, O 2 , air density, aerosol extinction and OClO. Nevertheless, OClO can not be retrieved using a single GOMOS measurement because of the weak signal-to-noise ratio and the small optical thickness associated with this molecule. We present here the method used to detect this molecule by using several GOMOS measurements. It is based on a two-step approach. First, several co-located measurements are combined in a statistical way to build an averaged measurement with a higher signal-to-noise ratio. Then, a Differential Optical Absorption Spectroscopy (DOAS) method is applied to retrieve OClO slant column densities. The statistics of the sets of GOMOS measurements used to build the averaged measurement and the spectral window selection are analyzed. The obtained retrievals are compared to results from two balloon-borne instruments. It appears that the inter-comparisons of OClO are generally satisfying. Then, two nighttime climatologies of OClO slant column densities based on GOMOS averaged measurements are presented. The first depicts annual global pictures of OClO from 2003 to 2011. From this climatology, the presence of an OClO layer in the equatorial region at about 35 km is confirmed and strong concentrations of OClO in both polar regions are observed, a sign of chlorine activation. The second climatology is a monthly time series. It clearly shows the chlorine activation of the lower stratosphere during winter. Moreover the equatorial OClO layer is observed during all the years without any significant variations. Finally, the anti-correlation between OClO and NO 2 is highlighted. This very promising method, applied on GOMOS measurements, allowed us to build the first nighttime climatology of OClO.