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This paper describes a neural network cloud masking scheme from PARASOL (Polarization and Anisotropy of Reflectances for Atmospheric Science coupled with Observations from a Lidar) multi-angle polarimetric measurements. The algorithm has been trained on synthetic measurements and has been applied to the processing of 1 year of PARASOL data. Comparisons of the retrieved cloud fraction with MODIS (Moderate Resolution Imaging Spectroradiometer) products show overall agreement in spatial and temporal patterns, but the PARASOL neural network (PARASOL-NN) retrieves lower cloud fractions. Comparisons with a goodness-of-fit mask from aerosol retrievals suggest that the NN cloud mask flags fewer clear pixels as cloudy than MODIS (∼ 3 % of the clear pixels versus ∼ 15 % by MODIS). On the other hand the NN classifies more pixels incorrectly as clear than MODIS (∼ 20 % by NN, versus ∼ 15 % by MODIS). Additionally, the NN and MODIS cloud mask have been applied to the aerosol retrievals from PARASOL using the Remote Sensing of Trace Gas and Aerosol Products (RemoTAP) algorithm. Validation with AERONET shows that the NN cloud mask performs comparably with MODIS in screening residual cloud contamination in retrieved aerosol properties. Our study demonstrates that cloud masking from multi-angle polarimeter (MAP) aerosol retrievals can be performed based on the MAP measurements themselves, making the retrievals independent of the availability of a cloud imager. [ABSTRACT FROM AUTHOR]

From a passive satellite remote sensing point of view, the richest set of information on aerosol properties can be obtained from instruments that measure both intensity and polarization of backscattered sunlight at multiple wavelengths and multiple viewing angles for one ground pixel. However, it is challenging to exploit this information at a global scale because complex algorithms are needed with many fit parameters (aerosol and land/ocean reflection), based on online radiative transfer models. So far, two such algorithms have demonstrated this capability at a global scale: the Generalized Retrieval of Atmosphere and Surface Properties (GRASP) algorithm and the Remote sensing of Trace gas and Aerosol Products (RemoTAP) algorithm. In this paper, we present a detailed comparison of the most recent versions of RemoTAP and GRASP. We evaluate both algorithms for synthetic observations, for real PARASOL (Polarization and Anisotropy of Reflectances for Atmospheric Science coupled with Observations from a Lidar) observations against AERONET (Aerosol Robotic Network) for common pixels, and for global PARASOL retrievals for the year 2008. For the aerosol optical depth (AOD) over land, both algorithms show a root mean square error (RMSE) of 0.10 (at 550 nm). For single scattering albedo (SSA), both algorithms show a good performance in terms of RMSE (0.04), but RemoTAP has a smaller bias (0.002) compared to GRASP (0.021). For the Ångström exponent (AE), GRASP has a smaller RMSE (0.367) than RemoTAP (0.387), mainly caused by a small overestimate of AE at low values (large particles). Over ocean both algorithms perform very well. For AOD, RemoTAP has an RMSE of 0.057 and GRASP an even smaller RMSE of 0.047. For AE, the RMSEs of RemoTAP and GRASP are 0.285 and 0.224, respectively. Based on the AERONET comparison, we conclude that both algorithms show very similar overall performance, where both algorithms have stronger and weaker points. For the global data products, we find a root mean square difference (RMSD) between RemoTAP and GRASP AOD of 0.12 and 0.038 over land and ocean, respectively. The largest differences occur over the biomass burning region in equatorial Africa. The global mean values are virtually unbiased with respect to each other. For AE the RMSD between RemoTAP and GRASP is 0.33 over land and 0.23 over ocean. For SSA, we find much better agreement over land (bias = - 0.01, RMSD = 0.043 for retrievals with AOD > 0.2) than over ocean (bias = 0.053, RMSD = 0.074). As expected, the differences increase towards low AOD, over both land and ocean. We also compared the GRASP and RemoTAP AOD and AE products against MODIS. For AOD over land, the agreement of either GRASP or RemoTAP with MODIS is worse than the agreement between the two PARASOL algorithms themselves. Over ocean, the agreement is very similar among the three products for AOD. For AE, the agreement between GRASP and RemoTAP is much better than the agreement of both products with MODIS. The agreement of the latest product versions with each other and with AERONET improved significantly compared to the previous version of the global products of GRASP and RemoTAP. The results demonstrate that the dedicated effort in algorithm development for multi-angle polarimetric (MAP) aerosol retrievals still leads to substantial improvement of the resulting aerosol products, and this is still an ongoing process. [ABSTRACT FROM AUTHOR]

Uncrewed aerial vehicles (UAVs) have become widely used in a range of atmospheric science research applications. Because of their small size, flexible range of motion, adaptability, and low cost, multirotor UAVs are especially well-suited for probing the lower atmosphere. However, their use so far has been limited to conditions outside of clouds, first because of the difficulty of flying beyond visual line of sight and second because of the challenge of flying in icing conditions in supercooled clouds. Here, we present two UAVs for cloud microphysical research: one UAV (the measurement UAV) equipped with a Portable Optical Particle Spectrometer (POPS) and meteorological sensors to probe the aerosol and meteorological properties in the boundary layer and one UAV (the seeding UAV) equipped with seeding flares to produce a plume of particles that can nucleate ice in supercooled clouds. A propeller heating mechanism on both UAVs allows for operating in supercooled clouds with icing conditions. These UAVs are an integral part of the CLOUDLAB project in which glaciogenic cloud seeding of supercooled low stratus clouds is utilized for studying aerosol–cloud interactions and ice crystal formation and growth. In this paper, we first show validations of the POPS on board the measurement UAV, demonstrating that the rotor turbulence has a small effect on measured particle number concentrations. We then exemplify the applicability for profiling the planetary boundary layer, as well as for sampling and characterizing aerosol plumes, in this case, the seeding plume. We also present a new method for filtering out high-concentration data to ensure good data quality of POPS. We explain the different flight patterns that are possible for both UAVs, namely horizontal or vertical leg patterns or hovering, with an extensive and flexible parameter space for designing the flight patterns according to our scientific goals. Finally, we show two examples of seeding experiments: first characterizing an out-of-cloud seeding plume with the measurement UAV flying horizontal transects through the plume and, second, characterizing an in-cloud seeding plume with downstream measurements from a POPS and a holographic imager mounted on a tethered balloon. Particle number concentrations and particle number size distributions of the seeding plume from the experiments reveal that we can successfully produce and measure the seeding plume, both in-cloud (with accompanying elevated ice crystal number concentrations) and out-of-cloud. The methods presented here will be useful for probing the lower atmosphere, for characterizing aerosol plumes, and for deepening our cloud microphysical understanding through cloud seeding experiments, all of which have the potential to benefit the atmospheric science community. [ABSTRACT FROM AUTHOR]

Here we present first Eddy Covariance (EC) measurements of fluxes of glyoxal, the smallest α-dicarbonyl product of hydrocarbon oxidation, and a precursor for secondary organic aerosol (SOA). The unique physical and chemical properties of glyoxal, i.e., high solubility in water (Henry's Law constant, KH =4.2 × 105Matm-1) and short atmospheric lifetime (∼2 h at solar noon) make it a unique indicator species for organic carbon oxidation in the marine atmosphere. Previous reports of elevated glyoxal over oceans remain unexplained by atmospheric models. Here we describe a Fast Light Emitting Diode Cavity Enhanced Differential Optical Absorption Spectroscopy (Fast LED-CE-DOAS) instrument to measure diurnal variations and EC fluxes of glyoxal, and inform about its unknown sources. The fast in situ sensor is described, and first results are presented from a cruise deployment over the Eastern tropical Pacific Ocean (20° N to 10° S; 133° W to 85° W) as part of the Tropical Ocean Troposphere Exchange of Reactive Halogens and OVOC (TORERO) field experiment (January to March 2012). The Fast LED-CE-DOAS is a multispectral sensor that selectively and simultaneously measures glyoxal (CHOCHO), nitrogen dioxide (NO2), oxygen dimers (O4) and water vapor (H2O) with ∼2 Hz time resolution, and a precision of ∼40 pptv Hz-0.5 for glyoxal. The instrument is demonstrated to be a "white-noise" sensor suitable for EC flux measurements; further, highly sensitive and inherently calibrated glyoxal measurements are obtained from temporal averaging of data (∼2 pptv detection limit over 1 h). The campaign averaged mixing ratio in the Southern Hemisphere (SH) is found to be 43 ± 9 pptv glyoxal, and is higher than in the Northern Hemisphere (NH: 32 ±6 pptv; error reflects variability over multiple days). The diurnal variation of glyoxal in the MBL is measured for the first time, and mixing ratios vary by ∼8ppt (NH) and ∼12 pptv (SH) over the course of 24h. Consistently, maxima are observed at sunrise (NH: 35 ±5 pptv; SH: 47 ±7 pptv) and minima at dusk (NH: 27 ±5 pptv; SH: 35 ±8 pptv). Ours are the first EC flux measurements of glyoxal. In both hemispheres, the daytime flux was directed from the atmosphere into the ocean, indicating that the ocean is a net sink for glyoxal during the day. After sunset the ocean was a source for glyoxal to the atmosphere (posi?tive flux) in the SH; this primary ocean source was operative throughout the night. In the NH, the nighttime flux was positive only shortly after sunset, and negative during most of the night. Positive EC fluxes of soluble glyoxal over oceans indicate the presence of an ocean surface organic microlayer (SML), and locate a glyoxal source within the SML. The origin of atmospheric glyoxal, and possibly other oxygenated hydrocarbons over tropical oceans warrants further investigation. [ABSTRACT FROM AUTHOR]

The continued interest in air pollution and stratospheric ozone variability has motivated the development of a Geostationary Environmental Monitoring Spectrometer (GEMS) for hourly ozone monitoring. This paper provides the atmospheric science community with the world's first assessment of GEMS total column ozone (TCO) retrieval performance and diurnal ozone variation. The algorithm used for GEMS is a more advanced version of its predecessor, the Total Ozone Mapping Spectrometer (TOMS) V8, that incorporates several improvements, including a new lookup table, a simple Lambertian-equivalent reflectivity model, and a spectral dependence correction. The GEMS algorithm also uses the optimal estimation method (OEM) to make error analysis more accessible and robust. The estimated retrieval errors range from 1.5 to 2 DU in September and 2 DU in December, with a constant degree of freedom of the signal (DFS) of 1 in September and a variable DFS of 1.25 to 1.4 in December throughout the day, depending on solar zenith angle (SZA). To assess the performance of the GEMS algorithm, the hourly GEMS total ozone was compared with ground-based measurements from Pandora instruments and other satellite platforms from TROPOMI (TROPOspheric Monitoring Instrument) and OMPS (Ozone Mapping and Profiler Suite Nadir Mapper). GEMS has a high correlation of 0.97 and small RMSE values compared to Pandora TCO at Busan and Seoul in South Korea. It is notable that despite exhibiting seasonal dependence in the mean bias of GEMS with Pandora, GEMS is capable of observing daily variations in ozone that are highly consistent with Pandora measurements, with a bias of approximately 1 %. The comparison of GEMS TCO data with TROPOMI and OMPS TCO data shows a high correlation of 0.99 and low RMSE compared to TROPOMI and OMPS TCO data, but the data have a negative bias of -2.38 % and -2.17 %, with standard deviations of 1.33 % and 1.57 %, respectively. Similar to OMPS, the influence of SO 2 from volcanic eruptions is not properly removed in some regions, leading to GEMS overestimating TCO in those areas. The mean biases of GEMS TCO data with TROPOMI and OMPS TCO are within ±1 % at low latitudes but become negative at midlatitudes, with an increasingly negative dependence on latitude. Furthermore, this dependence becomes more prominent from summer to winter. The empirical correction applied to the GEMS irradiance data improves the dependence of the mean bias on season and latitude, but a consistent bias still remains, and a marginal positive trend was observed in December. Therefore, further investigation into correction methods is needed. The results are a meaningful scientific advance by providing the first validated, hourly UV ozone retrievals from a satellite in geostationary orbit. This experience can be used to advance research with future geostationary environmental satellite missions, including the incoming TEMPO (Tropospheric Emissions: Monitoring of Pollution) and Sentinel-4. [ABSTRACT FROM AUTHOR]

For the last 25 years, CO-PDD (Cézeaux-Aulnat-Opme-puy de Dôme) has evolved to become a full instrumented platform for atmospheric research. It has received credentials as a national observing platform in France and is internationally recognized as a global station in the GAW (Global Atmosphere Watch) network. It is a reference site of European and national research infrastructures ACTRIS (Aerosol Cloud and Trace gases Research Infrastructure) and ICOS (Integrated Carbon Observing System). The site located on top of the puy de Dôme mountain (1465 m a.s.l.) is completed by additional sites located at lower altitudes and adding the vertical dimension to the atmospheric observations: Opme (660 m a.s.l.), Cézeaux (410 m), and Aulnat (330 m). The integration of different sites offers a unique combination of in situ and remote sensing measurements capturing and documenting the variability of particulate and gaseous atmospheric composition, but also the optical, biochemical, and physical properties of aerosol particles, clouds, and precipitations. Given its location far away from any major emission sources, its altitude, and the mountain orography, the puy de Dôme station is ideally located to sample different air masses in the boundary layer or in the free troposphere depending on time of day and seasons. It is also an ideal place to study cloud properties with frequent presence of clouds at the top in fall and winter. As a result of the natural conditions prevailing at the site and of the very exhaustive instrumental deployment, scientific studies at the puy de Dôme strongly contribute to improving knowledge in atmospheric sciences, including the characterization of trends and variability, the understanding of complex and interconnected processes (microphysical, chemical, biological, chemical and dynamical), and the provision of reference information for climate/chemistry models. In this context, CO-PDD is a pilot site to conduct instrumental development inside its wind tunnel for testing liquid and ice cloud probes in natural conditions, or in situ systems to collect aerosol and cloud. This paper reviews 25 years (1995–2020) of atmospheric observation at the station and related scientific research contributing to atmospheric and climate science. [ABSTRACT FROM AUTHOR]

This paper presents the physical basis of the Earth Polychromatic Imaging Camera (EPIC) cloud product algorithms and an initial evaluation of their performance. Since June 2015, EPIC has been providing observations of the sunlit side of the Earth with its 10 spectral channels ranging from the UV to the near-infrared. A suite of algorithms has been developed to generate the standard EPIC Level 2 cloud products that include cloud mask, cloud effective pressure/height, and cloud optical thickness. The EPIC cloud mask adopts the threshold method and utilizes multichannel observations and ratios as tests. Cloud effective pressure/height is derived with observations from the O2 A-band (780 and 764 nm) and B-band (680 and 688 nm) pairs. The EPIC cloud optical thickness retrieval adopts a single-channel approach in which the 780 and 680 nm channels are used for retrievals over ocean and over land, respectively. Comparison with co-located cloud retrievals from geosynchronous earth orbit (GEO) and low earth orbit (LEO) satellites shows that the EPIC cloud product algorithms are performing well and are consistent with theoretical expectations. These products are publicly available at the Atmospheric Science Data Center at the NASA Langley Research Center for climate studies and for generating other geophysical products that require cloud properties as input. [ABSTRACT FROM AUTHOR]

This paper describes a neural network algorithm for the estimation of liquid water cloud optical properties from the Polarization and Directionality of Earth's Reflectances-3 (POLDER-3) instrument aboard the Polarization & Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL) satellite. The algorithm has been trained on synthetic multi-angle, multi-wavelength measurements of reflectance and polarization and has been applied to the processing of 1 year of POLDER-3 data. Comparisons of the retrieved cloud properties with Moderate Resolution Imaging Spectroradiometer (MODIS) products show that the neural network algorithm has a low bias of around 2 in cloud optical thickness (COT) and between 1 and 2 µ m in the cloud effective radius. Comparisons with existing POLDER-3 datasets suggest that the proposed scheme may have enhanced capabilities for cloud effective radius retrieval, at least over land. An additional feature of the presented algorithm is that it provides COT and effective radius retrievals at the native POLDER-3 Level 1B pixel level. [ABSTRACT FROM AUTHOR]

This paper describes the Radio Occultation Processing Package, ROPP, a product of the EUMETSAT Radio Occultation Meteorology Satellite Application Facility (ROM SAF) developed by a large number of scientists over many years. A brief review of the concepts, functionality and structure of ROPP is followed by more detailed descriptions of its key capabilities. Example results from a full chain of processing using some of the ROPP tools are presented. Some current and prospective uses of ROPP are given. Instructions on how to access the code and its supporting documentation are provided. [ABSTRACT FROM AUTHOR]

Instruments measuring aerosol light absorption, such as the Aethalometer and the Multi-Wavelength Absorbance Analyzer (MWAA), have been extensively used to characterize optical absorption of atmospheric particulate matter. Data retrieved with such instruments can be analysed with mathematical models to apportion different aerosol sources (Aethalometer model) and components (MWAA model). In this work we present an upgrade to the MWAA optical apportionment model. In addition to the apportionment of the absorption coefficient babs in its components (black carbon and brown carbon) and sources (fossil fuels and wood burning), the extended model allows for the retrieval of the absorption Ångström exponent of each component and source, thereby avoiding initial assumptions regarding these parameters. We also present a new open-source software toolkit, the MWAA model toolkit (MWAA_MT), written in both Python and R, that performs the entire apportionment procedure. [ABSTRACT FROM AUTHOR]

In order to conduct accurate aerosol retrieval over snow, the Remote Sensing of Trace Gases and Aerosol Products (RemoTAP) algorithm developed by SRON Netherlands Institute for Space Research is extended with a bi-directional reflection distribution function (BRDF) for snow surfaces. The capability of the extended algorithm is validated with both synthetic measurements and real satellite measurements from the Polarization & Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL), and a comparison has been made to retrievals with the baseline RemoTAP (without a snow kernel). For retrievals with real PARASOL observations, we use pixels over Aerosol Robotic Network (AERONET) stations for validation and we use the MODIS snow cover products to identify pixels over snow. We evaluate the retrieved aerosol optical thickness (AOT) at 550 nm (τ550) , single-scattering albedo (SSA) at 550 nm (ω550) and Ångström exponent (AE) for 440–870 nm (AE440-870). The experiments with both synthetic and real data show that the extended RemoTAP maintains capability for snow-free pixels and has obvious advantages in accuracy and the fraction of successful retrievals for retrieval over snow, especially over surfaces with snow cover >75 %. According to the real-data experiment, we find that the retrieval algorithm has difficulty in fitting the PARASOL 1020 nm band, where snow reflectance is significantly lower than that for the visible bands. When we perform a four-band retrieval (490, 565, 670, 865 nm) with the extended RemoTAP, we obtain a good retrieval result for τ550 , ω550 and AE440-870. Therefore, the four-band retrieval with the extended RemoTAP is recommended for aerosol retrieval over snow. [ABSTRACT FROM AUTHOR]

The upper troposphere/lower stratosphere (UTLS) represents an important part of the climate system. Even small changes in the composition and dynamic structure of this region have significant radiative effects. Quantifying the underlying physical and chemical processes therefore represents a crucial task. Currently, there is a lack of UTLS observations with sufficient three-dimensional resolution. The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) aircraft instrument addresses this observational lack by providing observations of numerous trace constituents as well as temperature and cloud structures with an unprecedented combination of vertical resolution (up to 300 m) and horizontal resolution (about 30km×30km). As a result, important scientific questions concerning stratosphere-troposphere exchange, the occurrence of subvisible cirrus clouds in the lowermost stratosphere (LMS), polar chemistry, and gravity wave processes can be addressed, as reviewed in this paper. [ABSTRACT FROM AUTHOR]

Hyperspectral radiance measurements in the oxygen A band are sensitive to the vertical distribution of atmospheric scatterers, which in principle allows the retrieval of 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 than 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. [ABSTRACT FROM AUTHOR]

The use of meteorological radars to study snowfall microphysical properties and processes is well established, in particular via a few distinct techniques: the use of radar polarimetry, of multi-frequency radar measurements, and of the radar Doppler spectra. We propose a novel approach to retrieve snowfall properties by combining the latter two techniques, while relaxing some assumptions on, e.g., beam alignment and non-turbulent atmosphere. The method relies on a two-step deep-learning framework inspired from data compression techniques: an encoder model maps a high-dimensional signal to a low-dimensional latent space, while the decoder reconstructs the original signal from this latent space. Here, Doppler spectrograms at two frequencies constitute the high-dimensional input, while the latent features are constrained to represent the snowfall properties of interest. The decoder network is first trained to emulate Doppler spectra from a set of microphysical variables, using simulations from the Passive and Active Microwave radiative TRAnsfer model (PAMTRA) as training data. In a second step, the encoder network learns the inverse mapping, from real measured dual-frequency spectrograms to the microphysical latent space; in doing so, it leverages with a convolutional structure the spatial consistency of the measurements to mitigate the ill-posedness of the problem. The method was implemented on X- and W-band data from the ICE GENESIS campaign that took place in the Swiss Jura Mountains in January 2021. An in-depth assessment of the retrieval accuracy was performed through comparisons with colocated aircraft in situ measurements collected during three precipitation events. The agreement is overall good and opens up possibilities for acute characterization of snowfall microphysics on larger datasets. A discussion of the sensitivity and limitations of the method is also conducted. The main contribution of this work is, on the one hand, the theoretical framework itself, which can be applied to other remote-sensing retrieval applications and is thus possibly of interest to a broad audience across atmospheric sciences. On the other hand, the seven retrieved microphysical descriptors provide relevant insights into snowfall processes. [ABSTRACT FROM AUTHOR]

This work presents results from an original open-source low-cost sensor (LCS) system developed to measure tropospheric O3 in a remote high altitude alpine site. Our study was conducted at the Col Margherita Observatory (2543 m above sea level), in the Italian Eastern Alps. The sensor system mounts three commercial low-cost O3/NO2 sensors that have been calibrated before field deployment against a laboratory standard (Thermo Scientific; 49i-PS), calibrated against the standard reference photometer no. 15 calibration scale of the World Meteorological Organization (WMO). Intra- and intercomparison between the sensors and a reference instrument (Thermo Scientific; 49c) have been conducted for 7 months from May to December 2018. The sensors required an individual calibration, both in laboratory and in the field. The sensor's dependence on the environmental meteorological variables has been considered and discussed. We showed that it is possible to reduce the bias of one LCS by using the average coefficient values of another LCS working in tandem, suggesting a way forward for the development of remote field calibration techniques. We showed that it is possible reconstruct the environmental ozone concentration during the loss of reference instrument data in situations caused by power outages. The evaluation of the analytical performances of this sensing system provides a limit of detection (LOD) <5 ppb (parts per billion), limit of quantification (LOQ) <17 ppb , linear dynamic range (LDR) up to 250 ppb , intra-Pearson correlation coefficient (PCC) up to 0.96 , inter-PCC >0.8 , bias >3.5 ppb and ±8.5 at 95 % confidence. This first implementation of a LCS system in an alpine remote location demonstrated how to obtain valuable data from a low-cost instrument in a remote environment, opening new perspectives for the adoption of low-cost sensor networks in atmospheric sciences. [ABSTRACT FROM AUTHOR]

The interplay of bio-aerosol dispersion and impact, meteorology, and air quality is gaining increasing interest in the wide spectrum of atmospheric sciences. Experiments conducted inside confined artificial environments, such as atmospheric simulation chambers (ASCs), where atmospheric conditions and composition are controlled, can provide valuable information on bio-aerosol viability, dispersion, and impact. We focus here on the reproducible aerosolization and injection of viable microorganisms into an ASC, the first and crucial step of any experimental protocol to expose bio-aerosols to different atmospheric conditions. We compare the performance of three nebulizers specifically designed for bio-aerosol applications: the Collison nebulizer, the Blaustein Atomizing Modules (BLAM), and the Sparging Liquid Aerosol Generator (SLAG), all manufactured and commercialized by CH TECHNOLOGIES. The comparison refers to operating conditions and the concentration of viable bacteria at the nebulizer outlet, with the final goal being to measure the reproducibility of the nebulization procedures and assess their application in experiments inside ASCs. A typical bacterial test model, Escherichia coli (ATCC® 25922™), was selected for such characterization. Bacteria suspensions with a concentration around 10 8 CFU mL -1 were first aerosolized at different air pressures and collected by a liquid impinger to obtain a correlation curve between airflow and nebulized bacteria for each generator. Afterwards, bacteria were aerosolized inside the atmospheric simulation chamber ChAMBRe (Chamber for Aerosol Modelling and Bio-aerosol Research) to measure the reproducibility of the whole procedure. An overall reproducibility of 11 % (i.e., standard deviation of the results obtained with the three nebulizers) was obtained with each nebulizer through a set of baseline experiments. [ABSTRACT FROM AUTHOR]

Carbonaceous aerosol is mainly composed of organic carbon (OC) and elemental carbon (EC). Both OC and EC originate from a variety of emission sources. Radiocarbon (14C) analysis can be used to apportion bulk aerosol, OC, and EC into their sources. However, such analyses require the physical separation of OC and EC. Here, we apply of ECT9 protocol to physically isolate OC and EC for 14C analysis and evaluate its effectiveness. Several reference materials are selected, including two pure OC (fossil "adipic acid" and contemporary "sucrose"), two pure EC (fossil "regal black" and "C1150"), and three complex materials containing contemporary and/or fossil OC and EC ("rice char", NIST urban dust standards "SRM1649a" and "SRM8785", i.e., fine fraction of resuspended SRM1649a on filters). The pure materials were measured for their OC, EC, and total carbon (TC) mass fractions and corresponding carbon isotopes to evaluate the uncertainty of the procedure. The average accuracy of TC mass, determined via volumetric injection of a sucrose solution, was approximately 5 %. Ratios of EC/TC and OC/TC were highly reproducible, with analytical precisions better than 2 % for all reference materials, ranging in size from 20 to 100 µg C. Consensus values were reached for all pure reference materials for both δ 13C and fraction modern (F14C), with an uncertainty of < 0.3 ‰ and approximately 5 %, respectively. The procedure introduced 1.3 ± 0.6 µg of extraneous carbon, an amount compatible to that of the Swiss_4S protocol. In addition, OC and EC were isolated from mixtures of pure contemporary OC (sucrose) with pure fossil EC (regal black) and fossil OC (adipic acid) with contemporary EC (rice char EC) to evaluate the effectiveness of OC and EC separation. Consensus F14C values were reached for all OC (∼ 5–30 µg) and EC (∼ 10–60 µg) fractions with an uncertainty of ∼ 5 % on average. We found that the ECT9 protocol efficiently isolates OC or EC from complex mixtures. Based on δ 13C measurements, the average contribution of charred OC to EC is likely less than 3 % when the OC loading amount is less than 30 µg C. Charring was further assessed by evaluating thermograms of various materials, including aerosol samples collected in the Arctic and from tailpipes of gasoline or diesel engines. These data demonstrate that the ECT9 method effectively removes pyrolyzed OC. Thus, the ECT9 protocol, initially developed for concentration and stable isotope measurements of OC and EC, is suitable for 14C -based apportionment studies, including µgC -sized samples from arctic environments. [ABSTRACT FROM AUTHOR]

In the frame of the EMEP/ACTRIS/COLOSSAL campaign in Milan during winter 2018, equivalent black carbon measurements using the Aethalometer 31 (AE31), the Aethalometer 33 (AE33), and a Multi-Angle Absorption Photometer (MAAP) were carried out together with levoglucosan analyses on 12 h resolved PM2.5 samples collected in parallel. From AE31 and AE33 data, the loading-corrected aerosol attenuation coefficients (bATN) were calculated at seven wavelengths (λ , where λ values are 370, 470, 520, 590, 660, 880, and 950 nm). The aerosol absorption coefficient at 637 nm (babs_MAAP) was determined by MAAP measurements. Furthermore, babs was also measured at four wavelengths (405, 532, 635, 780 nm) on the 12 h resolved PM2.5 samples by a polar photometer (PP_UniMI). After comparing PP_UniMI and MAAP results, we exploited PP_UniMI data to evaluate the filter multiple-scattering enhancement parameter at different wavelengths for AE31 and AE33. We obtained instrument- and wavelength-dependent multiple-scattering enhancement parameters by linear regression of the Aethalometer bATN against the babs measured by PP_UniMI. We found significant dependence of the multiple-scattering enhancement parameter on filter material, hence on the instrument, with a difference of up to 30 % between the AE31 and the AE33 tapes. The wavelength dependence and day–night variations were small – the difference between the smallest and largest value was up to 6 %. Data from the different instruments were used as input to the so-called "Aethalometer model" for optical source apportionment, and instrument dependence of the results was investigated. Inconsistencies among the source apportionment were found fixing the AE31 and AE33 multiple-scattering enhancement parameters to their usual values. In contrast, optimised multiple-scattering enhancement parameters led to a 5 % agreement among the approaches. Also, the component apportionment "MWAA model" (Multi-Wavelength Absorption Analyzer model) was applied to the dataset. It was less sensitive to the instrument and the number of wavelengths, whereas significant differences in the determination of the absorption Ångström exponent for brown carbon were found (up to 22 %). [ABSTRACT FROM AUTHOR]

The Orbitrap mass spectrometer has recently been proved to be a powerful instrument to accurately measure gas-phase and particle-phase organic compounds with a greater mass resolving power than other widely used online mass spectrometers in atmospheric sciences. We develop an open-source software tool (Orbitool, https://orbitrap.catalyse.cnrs.fr , last access: 4 February 2021) to facilitate the analysis of long-term online Orbitrap data. Orbitool can average long-term data while improving the mass accuracy by re-calibrating each mass spectrum, assign molecular formulae of compounds and their isotopes to measured signals, and export time series and mass defect plots. The noise reduction procedure in Orbitool can separate signal peaks from noise and reduce the computational and storage expenses. Chemical ionization Orbitrap data from laboratory experiments on ozonolysis of monoterpenes and ambient measurements in urban Shanghai were used to test Orbitool. For the test dataset, the average mass accuracy was improved from <2 to <0.5 ppm by mass calibrating each spectrum. The denoising procedure removed 97 % of the noise peaks from a spectrum averaged for 30 min while maintaining the signal peaks, substantially helping the automatic assignment of unknown species. To illustrate the capabilities of Orbitool, we used the most challenging and complex dataset we have collected so far, which consists of ambient gas-phase measurements in urban Shanghai. These tests showed that Orbitool was able to automatically assign hundreds of molecular formulae as well as their isotopes with high accuracy. [ABSTRACT FROM AUTHOR]

Smartphones are increasingly being equipped with atmospheric measurement sensors providing huge auxiliary resources for global observations. Although China has the highest number of cell phone users, there is little research on whether these measurements provide useful information for atmospheric research. Here, for the first time, we present the global spatial and temporal variation in smartphone pressure measurements collected in 2016 from the Moji Weather app. The data have an irregular spatiotemporal distribution with a high density in urban areas, a maximum in summer and two daily peaks corresponding to rush hours. With the dense dataset, we have developed a new bias-correction method based on a machine-learning approach without requiring users' personal information, which is shown to reduce the bias of pressure observation substantially. The potential application of the high-density smartphone data in cities is illustrated by a case study of a hailstorm that occurred in Beijing in which high-resolution gridded pressure analysis is produced. It is shown that the dense smartphone pressure analysis during the storm can provide detailed information about fine-scale convective structure and decrease errors from an analysis based on surface meteorological-station measurements. This study demonstrates the potential value of smartphone data and suggests some future research needs for their use in atmospheric science. [ABSTRACT FROM AUTHOR]

The aerosol fine-mode fraction (FMF) is an important optical parameter of aerosols, and the FMF is difficult to accurately retrieve by traditional satellite remote sensing methods. In this study, FMF retrieval was carried out based on the multiangle polarization data of Polarization and Anisotropy of Reflectances for Atmospheric Science coupled with Observations from Lidar (PARASOL), which overcame the shortcomings of the FMF retrieval algorithm in our previous research. In this research, FMF retrieval was carried out in China and compared with the AErosol RObotic NETwork (AERONET) ground-based observation results, Moderate Resolution Imaging Spectroradiometer (MODIS) FMF products, and Generalized Retrieval of Aerosol and Surface Properties (GRASP) FMF results. In addition, the FMF retrieval algorithm was applied, a new FMF dataset was produced, and the annual and quarterly average FMF results from 2006 to 2013 were obtained for all of China. The research results show that the FMF retrieval results of this study are comparable with the AERONET ground-based observation results in China and the correlation coefficient (r), mean absolute error (MAE), root mean square error (RMSE), and the proportion of results that fall within the expected error (Within EE) are 0.770, 0.143, 0.170, and 65.01 %, respectively. Compared with the MODIS FMF products, the FMF results of this study are closer to the AERONET ground-based observations. Compared with the FMF results of GRASP, the FMF results of this study are closer to the spatial variation in the ratio of PM 2.5 to PM 10 near the ground. [ABSTRACT FROM AUTHOR]

Proton-transfer-reaction mass spectrometry (PTR-MS) is widely used in atmospheric sciences for measuring volatile organic compounds in real time. In the most widely used type of PTR-MS instruments, air is directly introduced into a chemical ionization reactor via an inlet capillary system. The reactor has a volumetric exchange time of ∼0.1 s, enabling PTR-MS analyzers to measure at a frequency of 10 Hz. The time response does, however, deteriorate if low-volatility analytes interact with surfaces in the inlet or in the instrument. Herein, we present the extended volatility range (EVR) PTR-MS instrument which mitigates this issue. In the EVR configuration, inlet capillaries are made of passivated stainless steel, and all wetted metal parts in the chemical ionization reactor are surface-passivated with a functionalized hydrogenated amorphous silicon coating. Heating the entire setup (up to 120 ∘ C) further improves the time-response performance. We carried out time-response performance tests on a set of 29 analytes having saturation mass concentrations C0 in the range between 10-3 and 105 µgm-3. The 1/e -signal decay times after instant removal of the analyte from the sampling flow were between 0.2 and 90 s for gaseous analytes. We also tested the EVR PTR-MS instrument in combination with the chemical analysis of aerosols online (CHARON) particle inlet, and 1/e -signal decay times were in the range between 5 and 35 s for particulate analytes. We show on a set of example compounds that the time-response performance of the EVR PTR-MS instrument is comparable to that of the fastest flow tube chemical ionization mass spectrometers that are currently in use. The fast time response can be used for rapid (∼1 min equilibration time) switching between gas and particle measurements. The CHARON EVR PTR-MS instrument can thus be used for real-time monitoring of both gaseous and particulate organics in the atmosphere. Finally, we show that the CHARON EVR PTR-MS instrument also rapidly detects highly oxygenated species (with up to eight oxygen atoms) in particles formed by limonene ozonolysis. [ABSTRACT FROM AUTHOR]

Correct, timely and meaningful interpretation of polarimetric weather radar observations requires an accurate understanding of hydrometeors and their associated microphysical processes along with well-developed techniques that automatize their recognition in both the spatial and temporal dimensions of the data. This study presents a novel technique for identifying different types of hydrometeors from quasi-vertical profiles (QVPs). In this new technique, the hydrometeor types are identified as clusters belonging to a hierarchical structure. The number of different hydrometeor types in the data is not predefined, and the method obtains the optimal number of clusters through a recursive process. The optimal clustering is then used to label the original data. Initial results using observations from the National Centre for Atmospheric Science (NCAS) X-band dual-polarization Doppler weather radar (NXPol) show that the technique provides stable and consistent results. Comparison with available airborne in situ measurements also indicates the value of this novel method for providing a physical delineation of radar observations. Although this demonstration uses NXPol data, the technique is generally applicable to similar multivariate data from other radar observations. [ABSTRACT FROM AUTHOR]

In this study, we introduce a newly developed upper-air observational instrument for atmospheric research. The "Storm Tracker" is an ultra-lightweight (about 20 g including battery), multi-channel simultaneous capable radiosonde designed by the Department of Atmospheric Sciences at National Taiwan University. Developed in 2016, the Storm Tracker aims to provide an alternative for observing atmospheric vertical profiles with a high temporal resolution, especially the lower-level atmosphere under severe weather conditions such as extreme thunderstorms and tropical cyclones. Field experiments were conducted as trial runs in Wu-Chi, Taichung, Taiwan, to examine the ability of the Storm Tracker to observe the boundary layer, in addition to the intercomparison between the Storm Tracker and the widely used Vaisala RS41-SGP radiosonde. Among the co-launches of the Storm Tracker and Vaisala RS41 radiosondes, the measurements of pressure, wind speed, and wind direction are highly consistent between the measurements of the Storm Tracker and the Vaisala RS41-SGP. However, a significant daytime warm bias in the Storm Tracker was found due to solar heating. A metal shield specifically for the Storm Tracker was thus installed and showed mitigation for the warm biases and the overall variance. With the much lower costs of the radiosondes and the simultaneous multi-channel receiver, the Storm Tracker system has shown great potential for high-frequency observational needs in atmospheric research. [ABSTRACT FROM AUTHOR]

Source apportionment of organic aerosol (OA) from aerosol mass spectrometer (AMS) or aerosol chemical speciation monitor (ACSM) measurements relies largely upon mass spectral profiles from different source emissions. However, the changes in mass spectra of primary emissions from AMS–ACSM with the newly developed capture vaporizer (CV) are poorly understood. Here we conducted 21 cooking, crop straw, wood, and coal burning experiments to characterize the mass spectral features of OA and water-soluble OA (WSOA) using SV-AMS and CV-ACSM. Our results show overall similar spectral characteristics between SV-AMS and CV-ACSM for different primary emissions despite additional thermal decomposition in CV, and the previous spectral features for diagnostics of primary OA factors are generally well retained. However, the mass spectral differences between OA and WSOA can be substantial for both SV-AMS and CV-ACSM. The changes in f55 (fraction of m/z 55 in OA) vs. f57 , f44 vs. f60 , and f44 vs. f43 in CV-ACSM are also observed, yet the evolving trends are similar to those of SV-AMS. By applying the source spectral profiles to a winter CV-ACSM study at a highly polluted rural site in the North China Plain, the source apportionment of primary OA was much improved, highlighting the two most important primary sources of biomass burning and coal combustion (32 % and 21 %). Considering the rapidly increasing deployments of CV-ACSM and WSOA studies worldwide, the mass spectral characterization has significant implications by providing essential constraints for more accurate source apportionment and making better strategies for air pollution control in regions with diverse primary emissions. [ABSTRACT FROM AUTHOR]

Black carbon (BC) or soot is a constituent of particulate matter (PM) which is relevant for negative human health and climate effects, and despite the lack of direct legal limits, it is recognised as an important atmospheric pollutant to monitor, understand, and control. Aethalometers are instruments which continuously monitor BC by measuring absorption at a number of distinct wavelengths. If collocated elemental carbon (EC) observations are used to transform these values into BC mass, by convention, the result is named equivalent black carbon (EBC). BC emitted by different combustion processes has different optical absorption characteristics, and this can be used to apportion EBC mass into traffic (EBCTR) and woodburning (EBCWB) components with a data processing technique known as the aethalometer model. The aethalometer model was applied to six EBC monitoring sites across Switzerland (using data between 2008 and 2018) and was evaluated by investigating diurnal cycles, model coefficients, and ambient temperature dependence of the two EBC components. For one monitoring site, San Vittore, the aethalometer model failed to produce plausible outputs. The reason for this failure was likely due to a high load of freshly emitted wood smoke during the winter which should be thought of as a third distinct emission source. After model evaluation, the trend analysis indicated that EBCTR concentrations at the remaining five locations significantly decreased between 2008 and 2018. EBCWB also demonstrated significant decreases in most monitoring locations but not at a monitoring site south of the Alps with a high PM load sourced from biomass burning. Ratios of EBC and particulate matter with a diameter of less than 2.5 µm (PM 2.5) suggested that EBC contributes 6 %–14 % of the PM 2.5 mass in Switzerland. The aethalometer model is a useful data analysis procedure but can fail under certain conditions; thus, careful evaluation is required to ensure the method is robust and suitable in other locations. [ABSTRACT FROM AUTHOR]

The Multi-angle Imaging SpectroRadiometer (MISR) instrument has been operational on the National Aeronautics and Space Administration (NASA) Earth Observing System (EOS) Terra satellite since early 2000, creating an extensive data set of global Earth observations. Here we introduce the latest version of the MISR aerosol products. The level 2 (swath) product, which is reported on a 4.4 km spatial grid, is designated as version 23 (V23) and contains retrieved aerosol optical depth (AOD) and aerosol particle property information derived from MISR's multi-angle observations over both land and water. The changes from the previous version of the algorithm (V22) have significant impacts on the data product and its interpretation. The V23 data set is created from two separate retrieval algorithms that are applied over dark water and land surfaces, respectively. Besides increasing the horizontal resolution to 4.4 km compared with the coarser 17.6 m resolution in V22 and streamlining the format and content, the V23 product has added geolocation information, pixel-level uncertainty estimates, and improved cloud screening. MISR data can be obtained from the NASA Langley Research Center Atmospheric Science Data Center at https://eosweb.larc.nasa.gov/project/misr/misr%5ftable (last access: 11 October 2019). The version number for the V23 level 2 aerosol product is F13_0023. The level 3 (gridded) aerosol product is still reported at 0.5∘×0.5∘ spatial resolution with results aggregated from the higher-resolution level 2 data. The format and content at level 3 have also been updated to reflect the changes made at level 2. The level 3 product associated with the V23 level 2 product version is designated as F15_0032. Both the level 2 and level 3 products are now provided in NetCDF format. [ABSTRACT FROM AUTHOR]

Herein we report on the first successful airborne deployment of the CHemical Analysis of AeRosol ONline (CHARON) particle inlet which allowed us to measure the chemical composition of atmospheric submicrometer particles in real time using a state-of-the-art proton-transfer-reaction time-of-flight mass spectrometry (PTR-ToF-MS) analyzer. The data were collected aboard the NASA DC-8 Airborne Science Laboratory on 26 June 2018 over California in the frame of NASA's Student Airborne Research Program (SARP). We show exemplary data collected when the airplane (i) shortly encountered a fresh (<1 h old) smoke plume that had emanated from the Lions Fire in the Sierra Nevada, (ii) intercepted a particle plume emitted from an amine gas treating unit of a petroleum refinery close to Bakersfield, (iii) carried out a spatial survey in the boundary layer over the San Joaquin Valley and (iv) performed a vertical profile measurement over the greater Bakersfield area. The most important finding from this pilot study is that the CHARON PTR-ToF-MS system measures fast enough to be deployed on a jet research aircraft. The data collected during 3 to 15 s long plume encounters demonstrate the feasibility of airborne point or small area emission measurements. Further improvements are, however, warranted to eliminate or reduce the observed signal tailing (1/e decay time between 6 and 20 s). The fast time response of the analyzer allowed us to generate highly spatially resolved maps (1–2 km in the horizontal, 100 m in the vertical) of atmospheric particle chemical constituents. The chemical information that was extracted from the recorded particle mass spectra includes (i) mass concentrations of ammonium, nitrate and total organics; (ii) mass concentrations of different classes of organic compounds (CH vs. CHO vs. CHN vs. CHNO compounds; monoaromatic vs. polyaromatic compounds); (iii) aerosol bulk average O:C‾ and H:C‾ ratios; (iv) mass concentrations of selected marker molecules (e.g., levoglucosan in particles emitted from a wildfire, an alkanolamine in particles emitted from a petroleum refinery) and (v) wildfire emission ratios (Δ total organics/ Δ CO = 0.054; Δ levoglucosan/ Δ CO = 7.9×10-3 ; Δ vanillic acid/ Δ CO = 4.4×10-4 and Δ retene/ Δ CO = 1.9×10-4 ; all calculated as peak area ratios, in grams per gram). The capability of the CHARON PTR-ToF-MS instrument to chemically characterize submicrometer atmospheric particles in a quantitative manner, at the near-molecular level, and in real time brings a new and unprecedented measurement capability to the airborne atmospheric science community. [ABSTRACT FROM AUTHOR]

Two approaches are commonly used to simulate atmospheric aging processes in the laboratory. The experiments are either performed in large aerosol chambers (several m 3) in order to achieve extended observation times or in small chambers (< 1 m 3), compensating for the short observation times by elevated reactant concentrations. We present an experimental approach that enables long observation times at atmospherically relevant reactant concentrations in small chamber volumes by operating the aerosol chamber as a continuous-flow stirred tank reactor (CSTR). We developed a mathematical framework that allows the retrieval of data beyond calculating mean values, such as O3 exposure or equivalent atmospheric aging time, using the new metric, activation time (tact). This concept was developed and successfully tested to characterize the change in cloud condensation nuclei (CCN) activity of soot particles due to heterogeneous ozone oxidation. We found very good agreement between the experimental results and the theoretical predictions. This experimental approach and data analysis concept can be applied for the investigation of any transition in aerosol particles properties that can be considered a binary system. Furthermore, we show how tact can be applied to the analysis of data originating from other reactor types such as oxidation flow reactors (OFRs), which are widely used in atmospheric sciences. The new tact concept significantly supports the understanding of data acquired in OFRs, especially those from deviating experimental results in intercomparison campaigns. [ABSTRACT FROM AUTHOR]

In recent years, dual-polarisation Doppler X-band radars have become a widely used part of the atmospheric scientist's toolkit for examining cloud dynamics and microphysics and making quantitative precipitation estimates. This is especially true for research questions that require mobile radars. Here we describe the National Centre for Atmospheric Science (NCAS) mobile X-band dual-polarisation Doppler weather radar (NXPol) and the infrastructure used to deploy the radar and provide an overview of the technical specifications. It is the first radar of its kind in the UK. The NXPol is a Meteor 50DX manufactured by Selex-Gematronik (Selex ES GmbH), modified to operate with a larger 2.4 m diameter antenna that produces a 0.98 ∘ half-power beam width and without a radome. We provide an overview of the technical specifications of the NXPol with emphasis given to the description of the aspects of the infrastructure developed to deploy the radar as an autonomous observing facility in remote locations. To demonstrate the radar's capabilities, we also present examples of its use in three recent field campaigns and its ongoing observations at the NERC Facility for Atmospheric Radio Research (NFARR). [ABSTRACT FROM AUTHOR]

The sources and atmospheric chemistry of gasphase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. In this work, we evaluated the use of SF-6 as a sensitive and selective chemical ionization reagent ion for realtime measurements of gas-phase organic acids. Field measurements are made using chemical ionization mass spectrometry (CIMS) at a rural site in Yorkville, Georgia, from September to October 2016 to investigate the capability of this measurement technique. Our measurements demonstrate that SF-6 can be used to measure a range of organic acids in the atmosphere. One-hour averaged ambient concentrations of organic acids ranged from a few parts per trillion by volume (ppt) to several parts per billion by volume (ppb). All the organic acids displayed similar strong diurnal behaviors, reaching maximum concentrations between 17:00 and 19:00 EDT. The organic acid concentrations are dependent on ambient temperature, with higher organic acid concentrations being measured during warmer periods. [ABSTRACT FROM AUTHOR]

Since January 2004, the planetary Fourier spectrometer (PFS) on board the Mars Express satellite has been recording near-infrared limb spectra of high quality up to the tangent altitude 150 km, with potential information on density and thermal structure of the upper Martian atmosphere. We present first results of our modeling of the PFS short wavelength channel (SWC) daytime limb spectra for the altitude region above 90 km. We applied a ro-vibrational non-LTE model based on the stellar astrophysics technique of accelerated lambda iteration (ALI) to solve the multispecies and multi-level CO2 problem in the Martian atmosphere. We show that the long-standing discrepancy between observed and calculated spectra in the cores and wings of 4.3 μm region is explained by the non-thermal rotational distribution of molecules in the upper vibrational states 10011 and 10012 of the CO2 main isotope second hot (SH) bands above 90 km altitude. The redistribution of SH band intensities from band branch cores into their wings is caused (a) by intensive production of the CO2 molecules in rotational states with j > 30 due to the absorption of solar radiation in optically thin wings of 2.7 μm bands and (b) by a short radiative lifetime of excited molecules, which is insufficient at altitudes above 90 km for collisions to maintain rotation of excited molecules thermalized. Implications for developing operational algorithms for massive processing of PFS and other instrument limb observations are discussed. [ABSTRACT FROM AUTHOR]

We present a new methodology, which we call Single Pair of Observations Technique with Eddy Covariance (SPOT-EC), to estimate regional-scale surface fluxes of 222Rn from tower-based observations of 222Rn activity concentration, CO2 mole fractions and direct CO2 flux measurements from eddy covariance. For specific events, the regional (222Rn) surface flux is calculated from short-term changes in ambient (222Rn) activity concentration scaled by the ratio of the mean CO2 surface flux for the specific event to the change in its observed mole fraction. The resulting 222Rn surface emissions are integrated in time (between the moment of observation and the last prior background levels) and space (i.e. over the footprint of the observations). The measurement uncertainty obtained is about ±15 % for diurnal events and about ±10 % for longer-term (e.g. seasonal or annual) means. The method does not provide continuous observations, but reliable daily averages can be obtained. We applied our method to in situ observations from two sites in the Netherlands: Cabauw station (CBW) and Lutjewad station (LUT). For LUT, which is an intensive agricultural site, we estimated a mean 222Rn surface flux of (0.29 ± 0.02) atoms cm−2 s−1 with values  > 0.5 atoms cm−2 s−1 to the south and south-east. For CBW we estimated a mean 222Rn surface flux of (0.63 ± 0.04) atoms cm−2 s−1. The highest values were observed to the south-west, where the soil type is mainly river clay. For both stations good agreement was found between our results and those from measurements with soil chambers and two recently published 222Rn soil flux maps for Europe. At both sites, large spatial and temporal variability of 222Rn surface fluxes were observed which would be impractical to measure with a soil chamber. SPOT-EC, therefore, offers an important new tool for estimating regional-scale 222Rn surface fluxes. Practical applications furthermore include calibration of process-based 222Rn soil flux models, validation of atmospheric transport models and performing regional-scale inversions, e.g. of greenhouse gases via the SPOT 222Rn-tracer method. [ABSTRACT FROM AUTHOR]

Sentinel-5 (S5) and its precursor (S5P) are future European satellite missions aiming at global monitoring of methane (CH4) column-average dry air mole fractions (XCH4). The spectrometers to be deployed onboard the satellites record spectra of sunlight backscattered from the Earth's surface and atmosphere. In particular, they exploit CH4 absorption in the shortwave infrared spectral range around 1.65 µm (S5 only) and 2.35 µm (both S5 and S5P) wavelength. Given an accuracy goal of better than 2% for XCH4 to be delivered on regional scales, assessment and reduction of potential sources of systematic error such as spectroscopic uncertainties is crucial. Here, we investigate how spectroscopic errors propagate into retrieval errors on the global scale. To this end, absorption spectra of a groundbased Fourier transform spectrometer (FTS) operating at very high spectral resolution serve as estimate for the quality of the spectroscopic parameters. Feeding the FTS fitting residuals as a perturbation into a global ensemble of simulated S5- and S5P-like spectra at relatively low spectral resolution, XCH4 retrieval errors exceed 0.6% in large parts of the world and show systematic correlations on regional scales, calling for improved spectroscopic parameters. [ABSTRACT FROM AUTHOR]

In this study, we retrieve and document drizzle properties, and investigate the impact of drizzle on cloud property retrieval in Dong et al. (2014a) from ground-based measurements at the ARM Azores facility from June 2009 to December 2010. For the selected cloud and drizzle samples, the drizzle occurrence is 42.6%, with a maximum of 55.8% in winter and a minimum of 35.6% in summer. The annual means of drizzle liquid water path LWPd, effective radius rd, and number concentration Nd for the rain (virga) samples are 4.73 (1.25) gm-2, 61.5 (36.4) µm, and 0.38 (0.79) cm-3. The seasonal mean LWPd values are less than 3% of the LWP values retrieved by the microwave radiometer (MWR). The annual mean differences in cloud-droplet effective radius with and without drizzle are 0.75 and 2.35%, respectively, for the virga and rain samples. Therefore, we conclude that the impact of drizzle below the cloud base on cloud property retrieval is insignificant for a solar-transmission-based method, but significant for any retrievals using radar reflectivity. [ABSTRACT FROM AUTHOR]

High-precision analysis of the 17O/16O isotope ratio in water and water vapor is of interest in hydrological, paleoclimate, and atmospheric science applications. Of spe-cific interest is the parameter 17Oexcess (Δ17O), a measure of the deviation from a linear relationship between 17O/16Oand 18O/16O ratios. Conventional analyses of Δ17O of water are obtained by fluorination of H2O to O2 that is analyzed by dual-inlet isotope ratio mass spectrometry (IRMS).We describe a new laser spectroscopy instrument for high-precision Δ17O measurements. The new instrument uses cavity ring-down spectroscopy (CRDS) with laser-current-tuned cavity resonance to achieve reduced measurement drift compared with previous-generation instruments. Liquid water and water-vapor samples can be analyzed with a better than 8 per meg precision for Δ17O using integration times of less than 30min. Calibration with respect to accepted water standards demonstrates that both the precisionand the accuracy of Δ17O are competitive with conventional IRMS methods. The new instrument also achieves simultaneous analysis of δ18O, δ17O and δD with precision of< 0.03 ‰, < 0.02 and < 0.2‰, respectively, based on repeated calibrated measurements. [ABSTRACT FROM AUTHOR]

A compact (500 cm3), lightweight (500 g), nearfield, single particle backscattering optical spectrometer is described that mounts flush with the skin of an aircraft and measures the concentration and optical equivalent diameter of particles from 5 to 75 μm. The backscatter cloud probe (BCP) was designed as a real-time qualitative cloud detector primarily for data quality control of trace gas instruments developed for the climate monitoring instrument packages that are being installed on commercial passenger aircraft as part of the European Union In-Service Aircraft for a Global Observing System (IAGOS) program (http://www.iagos.org/). Subsequent evaluations of the BCP measurements on a number of research aircraft, however, have revealed it capable of delivering quantitative particle data products including size distributions, liquid-water content and other information on cloud properties. We demonstrate the instrument's capability for delivering useful long-term climatological, as well as aviation performance information, across a wide range of environmental conditions. The BCP has been evaluated by comparing its measurements with those from other cloud particle spectrometers on research aircraft and several BCPs are currently flying on commercial A340/A330 Airbus passenger airliners. The design and calibration of the BCP is described in this article, along with an evaluation of measurements made on the research and commercial aircraft. Preliminary results from more than 7000 h of airborne measurements by the BCP on two Airbus A340s operating on routine global traffic routes (one Lufthansa, the other China Airlines) show that more than 340 h of cloud data have been recorded at normal cruise altitudes (> 10 km) and more than 40% of the > 1200 flights were through clouds at some point between takeoff and landing. These data are a valuable contribution to databases of cloud properties, including sub-visible cirrus, in the upper troposphere and useful for validating satellite retrievals of cloud water and effective radius; in addition, providing a broader, geographically and climatologically relevant view of cloud microphysical variability that is useful for improving parameterizations of clouds in climate models. Moreover, they are also useful for monitoring the vertical climatology of clouds over airports, especially those over megacities where pollution emissions may be impacting local and regional climate. [ABSTRACT FROM AUTHOR]

Peak stratospheric chlorofluorocarbon (CFC) and other ozone depleting substance (ODS) concentrations were reached in the mid- to late 1990s. Detection and attribution of the expected recovery of the stratospheric ozone layer in an atmosphere with reduced ODSs as well as efforts to understand the evolution of stratospheric ozone in the presence of increasing greenhouse gases are key current research topics. These require a critical examination of the ozone changes with an accurate knowledge of the spatial (geographical and vertical) and temporal ozone response. For such an examination, it is vital that the quality of the measurements used be as high as possible and measurement uncertainties well quantified. In preparation for the 2014 United Nations Environment Programme (UNEP)/World Meteorological Organization (WMO) Scientific Assessment of Ozone Depletion, the SPARC/IO3C/IGACO-O3/NDACC (SI2N) Initiative was designed to study and document changes in the global ozone profile distribution. This requires assessing long-term ozone profile data sets in regards to measurement stability and uncertainty characteristics. The ultimate goal is to establish suitability for estimating long-term ozone trends to contribute to ozone recovery studies. Some of the data sets have been improved as part of this initiative with updated versions now available. This summary presents an overview of stratospheric ozone profile measurement data sets (ground and satellite based) available for ozone recovery studies. Here we document measurement techniques, spatial and temporal coverage, vertical resolution, native units and measurement uncertainties. In addition, the latest data versions are briefly described (including data version updates as well as detailing multiple retrievals when available for a given satellite instrument). Archive location information for each data set is also given. [ABSTRACT FROM AUTHOR]

In this study the temporal and spatial characteristics of the liquid water path (LWP) of low, middle and high level clouds are analysed using space-based observations from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) instrument onboard the Meteosat Second Generation 2 (MSG 2) satellite. Both geophysical quantities are part of the CLAAS (CLoud property dAtAset using SEVIRI) data set 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 during daylight conditions, associated with individual cloud types. We analysed the intrinsic variability of LWP, that is, the variability in only cloudy regions and the variations driven by cloud amount. The relative amplitude of the intrinsic diurnal cycle exceeded the cloud amount driven amplitude in our analysed cases. Our results reveal that each cloud type possesses a characteristic intrinsic LWP distribution. These frequency distributions are constant with time in the entire SEVIRI field of view, but vary for smaller regions like Central Europe. Generally the average LWP is higher over land than over sea; in the case of low clouds this amounts to 15-27%in 2009. The variance of the frequency distributions is enhanced as well. Also, the average diurnal cycle of LWP is related to cloud type with the most pronounced relative diurnal variations being detected for low and middle level clouds. Maps of the relative amplitude and the local time of maximum LWP show the variation throughout the SEVIRI field of view. [ABSTRACT FROM AUTHOR]

A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyser (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne operation. It was characterised in the laboratory with respect to instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation, a calibration strategy is described that utilises CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppb for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppb. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately determined and the uncertainty is estimated to be 12.4 ppb. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppb at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses. [ABSTRACT FROM AUTHOR]