Search Results
Increasing the spatial resolution of cloud property retrievals from Meteosat SEVIRI by use of its high-resolution visible channel: Evaluation of candidate approaches with MODIS observations
This study presents and evaluates several candidate approaches for downscaling observations from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) in order to increase the horizontal resolution of subsequent cloud optical thickness (τ) and effective droplet radius (reff) retrievals from the native ≈ 3km×3km spatial resolution of the narrowband channels to ≈ 1km×1km. These methods make use of SEVIRI's coincident broadband high-resolution visible (HRV) channel. For four example cloud fields, the reliability of each downscaling algorithm is evaluated by means of collocated 1km×1km MODIS radiances, which are reprojected to the horizontal grid of the HRV channel and serve as reference for the evaluation. By using these radiances, smoothed with the modulation transfer function of the native SEVIRI channels, as retrieval input, the accuracy at the SEVIRI standard resolution can be evaluated and an objective comparison of the accuracy of the different downscaling algorithms can be made. For the example scenes considered in this study, it is shown that neglecting high-frequency variations below the SEVIRI standard resolution results in significant random absolute deviations of the retrieved τ and reff of up to ≈ 14 and ≈ 6μm, respectively, as well as biases. By error propagation, this also negatively impacts the reliability of the subsequent calculation of liquid water path (WL) and cloud droplet number concentration (ND), which exhibit deviations of up to ≈ 89gm-2 and ≈ 177cm-3, respectively. For τ , these deviations can be almost completely mitigated by the use of the HRV channel as a physical constraint and by applying most of the presented downscaling schemes. Uncertainties in retrieved reff at the native SEVIRI resolution are smaller, and the improvements from downscaling the observations are less obvious than for τ. Nonetheless, the right choice of downscaling scheme yields noticeable improvements in the retrieved reff. Furthermore, the improved reliability in retrieved cloud products results in significantly reduced uncertainties in derived WL and ND. In particular, one downscaling approach provides clear improvements for all cloud products compared to those obtained from SEVIRI's standard resolution and is recommended for future downscaling endeavors. This work advances efforts to mitigate impacts of scale mismatches among channels of multiresolution instruments on cloud retrievals. © Author(s) 2020.
3+2 + X : what is the most useful depolarization input for retrieving microphysical properties of non-spherical particles from lidar measurements using the spheroid model of Dubovik et al. (2006)?
The typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β) at 355, 532, and 1064 nm and two extinction coefficients (α) at 355 and 532 nm. This data combination is referred to as a 3β C 2α or 3 + 2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter for the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of d that exceed 0.10 at 532 nm, i.e. in the presence of nonspherical particles such as desert dust, volcanic ash, and, under special circumstances, biomass-burning smoke. We use experimental data collected with instruments that are capable of measuring d at all three lidar wavelengths with an inversion routine that applies the spheroidal light-scattering model of Dubovik et al. (2006) with a fixed axis-ratio distribution to replicate scattering properties of non-spherical particles. The inversion gives the fraction of spheroids required to replicate the optical data as an additional output parameter. This is the first systematic test of the effect of using all theoretically possible combinations of d taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information of at least one wavelength already provides useful information for the inversion of optical data that have been collected in the presence of non-spherical mineral dust particles. However, any choice of d will give lower values of the single-scattering albedo than the traditional 3 + 2 data set. We find that input data sets that include d355 give a spheroid fraction that closely resembles the dust ratio we obtain from using β532 and d532 in a methodology applied in aerosol-type separation. The use of d355 in data sets of two or three d? reduces the spheroid fraction that is retrieved when using d532 and d1064. Use of the latter two parameters without accounting for d355 generally leads to high spheroid fractions that we consider not trustworthy. The use of three d instead of two δ, including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3 + 2 + d355 for the observations with varying contributions of mineral dust considered here. However, additional measurements at wavelengths different from 355 nm would be desirable for application to a wider range of aerosol scenarios that may include non-spherical smoke particles, which can have values of d355 that are indistinguishable from those found for mineral dust. We therefore conclude that - depending on measurement capability - the future standard input for inversion of lidar data taken in the presence of mineral dust particles and using the spheroid model of Dubovik et al. (2006) might be 3+2Cδ355 or 3 + 2 + δ355 + δ532. © 2019 The Author(s).
Polarization lidar: An extended three-signal calibration approach
We present a new formalism to calibrate a threesignal polarization lidar and to measure highly accurate height profiles of the volume linear depolarization ratios under realistic experimental conditions. The methodology considers elliptically polarized laser light, angular misalignment of the receiver unit with respect to the main polarization plane of the laser pulses, and cross talk among the receiver channels. A case study of a liquid-water cloud observation demonstrates the potential of the new technique. Long-term observations of the calibration parameters corroborate the robustness of the method and the long-term stability of the three-signal polarization lidar. A comparison with a second polarization lidar shows excellent agreement regarding the derived volume linear polarization ratios in different scenarios: A biomass burning smoke event throughout the troposphere and the lower stratosphere up to 16 km in height, a dust case, and also a cirrus cloud case. © Author(s) 2019.
Optimizing the detection, ablation, and ion extraction efficiency of a single-particle laser ablation mass spectrometer for application in environments with low aerosol particle concentrations
The aim of this study is to show how a newly developed aerodynamic lens system (ALS), a delayed ion extraction (DIE), and better electric shielding improve the efficiency of the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA). These improvements are applicable to single-particle laser ablation mass spectrometers in general. To characterize the modifications, extensive sizeresolved measurements with spherical polystyrene latex particles (PSL; 150-6000 nm) and cubic sodium chloride particles (NaCl; 400-1700 nm) were performed. Measurements at a fixed ALS position show an improved detectable particle size range of the new ALS compared to the previously used Liu-type ALS, especially for supermicron particles. At a lens pressure of 2.4 hPa, the new ALS achieves a PSL particle size range from 230 to 3240 nm with 50% detection efficiency and between 350 and 2000 nm with 95% detection efficiency. The particle beam divergence was determined by measuring the detection efficiency at variable ALS positions along the laser cross sections and found to be minimal for PSL at about 800 nm. Compared to measurements by singleparticle mass spectrometry (SPMS) instruments using Liutype ALSs, the minimum particle beam divergence is shifted towards larger particle sizes. However, there are no disadvantages compared to the Liu-type lenses for particle sizes down to 200 nm. Improvements achieved by using the DIE and an additional electric shielding could be evaluated by size-resolved measurements of the hit rate, which is the ratio of laser pulses yielding a detectable amount of ions to the total number of emitted laser pulses. In particular, the hit rate for multiply charged particles smaller than 500 nm is significantly improved by preventing an undesired deflection of these particles in the ion extraction field. Moreover, it was found that by using the DIE the ion yield of the ablation, ionization, and ion extraction process could be increased, resulting in up to 7 times higher signal intensities of the cation spectra. The enhanced ion yield results in a larger effective width of the ablation laser beam, which in turn leads to a hit rate of almost 100% for PSL particles in the size range from 350 to 2000 nm. Regarding cubic NaCl particles the modifications of the ALABAMA result in an up to 2 times increased detection efficiency and an up to 5 times increased hit rate. The need for such instrument modifications arises in particular for measurements of particles that are present in low number concentrations such as ice-nucleating particles (INPs) in general, but also aerosol particles at high altitudes or in pristine environments. Especially for these low particle number concentrations, improved efficiencies help to overcome the statistical limitations of single-particle mass spectrometer measurements. As an example, laboratory INP measurements carried out in this study show that the appli- cation of the DIE alone increases the number of INP mass spectra per time unit by a factor of 2 to 3 for the sampled substances. Overall, the combination of instrument modifications presented here resulted in an increased measurement efficiency of the ALABAMA for different particle types and particles shape as well as for highly charged particles. © 2020 Copernicus GmbH. All rights reserved.
Nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) for investigating hygroscopic properties of sub-10nm aerosol nanoparticles
Interactions between water and nanoparticles are relevant for atmospheric multiphase processes, physical chemistry, and materials science. Current knowledge of the hygroscopic and related physicochemical properties of nanoparticles, however, is restricted by the limitations of the available measurement techniques. Here, we present the design and performance of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. Detailed methods of calibration and validation are provided. Besides maintaining accurate and stable sheath and aerosol flow rates (1 %), high accuracy of the differential mobility analyzer (DMA) voltage (0:1 %) in the range of 0-50V is crucial for achieving accurate sizing and small sizing offsets between the two DMAs (1:4 %). To maintain a stable relative humidity (RH), the humidification system and the second DMA are placed in a well-insulated and air conditioner housing (0:1 K). We also tested and discussed different ways of preventing predeliquescence in the second DMA. Our measurement results for ammonium sulfate nanoparticles are in good agreement with Biskos et al. (2006b), with no significant size effect on the deliquescence and efflorescence relative humidity (DRH and ERH, respectively) at diameters down to 6 nm. For sodium sulfate nanoparticles, however, we find a pronounced size dependence of DRH and ERH between 20 and 6 nm nanoparticles. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
Characterization and first results from LACIS-T : a moist-air wind tunnel to study aerosol–cloud–turbulence interactions
The interactions between turbulence and cloud microphysical processes have been investigated primarily through numerical simulation and field measurements over the last 10 years. However, only in the laboratory we can be confident in our knowledge of initial and boundary conditions and are able to measure under statistically stationary and repeatable conditions. In the scope of this paper, we present a unique turbulent moist-air wind tunnel, called the Turbulent Leipzig Aerosol Cloud Interaction Simulator (LACIS-T) which has been developed at TROPOS in order to study cloud physical processes in general and interactions between turbulence and cloud microphysical processes in particular. The investigations take place under well-defined and reproducible turbulent and thermodynamic conditions covering the temperature range of warm, mixed-phase and cold clouds (25∘C>T>−40∘C ). The continuous-flow design of the facility allows for the investigation of processes occurring on small temporal (up to a few seconds) and spatial scales (micrometer to meter scale) and with a Lagrangian perspective. The here-presented experimental studies using LACIS-T are accompanied and complemented by computational fluid dynamics (CFD) simulations which help us to design experiments as well as to interpret experimental results. In this paper, we will present the fundamental operating principle of LACIS-T, the numerical model, and results concerning the thermodynamic and flow conditions prevailing inside the wind tunnel, combining both characterization measurements and numerical simulations. Finally, the first results are depicted from deliquescence and hygroscopic growth as well as droplet activation and growth experiments. We observe clear indications of the effect of turbulence on the investigated microphysical processes.
The potential of elastic and polarization lidars to retrieve extinction profiles
A new method, called ElEx (elastic extinction), is proposed for the estimation of extinction coefficient lidar profiles using only the information provided by the elastic and polarization channels of a lidar system. The method is applicable to lidar measurements both during daytime and nighttime under well-defined aerosol mixtures. ElEx uses the particle backscatter profiles at 532 nm and the vertically resolved particle linear depolarization ratio measurements at the same wavelength. The particle linear depolarization ratio and the lidar ratio values of pure aerosol types are also taken from literature. The total extinction profile is then estimated and compared well with Raman retrievals. In this study, ElEx was applied in an aerosol mixture of marine and dust particles at Finokalia station during the CHARADMExp campaign. Any difference between ElEx and Raman extinction profiles indicates that the nondust component could be probably attributed to polluted marine or polluted continental aerosols. Comparison with sun photometer aerosol optical depth observations is performed as well during daytime. Differences in the total aerosol optical depth are varying between 1.2 % and 72 %, and these differences are attributed to the limited ability of the lidar to correctly represent the aerosol optical properties in the near range due to the overlap problem. © 2020 Author(s).
Application of TXRF in monitoring trace metals in particulate matter and cloud water
Trace metals in ambient particulate matter and cloud are considered key elements of atmospheric processes as they affect air quality, environmental ecosystems, and cloud formation. However, they are often available at trace concentrations in these media such that their analysis requires high-precision and sensitive techniques. In this study, different analytical methods were applied to quantify trace metals in particulate matter (PM) samples collected on quartz and polycarbonate filters as well as cloud water, using the Total reflection X-Ray Fluorescence (TXRF) technique. These methods considered the measurement of filter samples directly without and with chemical pretreatment. Direct measurements involved the analysis of PM samples collected on polycarbonate filters and cloud water samples after they are brought onto TXRF carrier substrates. The chemical treatment method involved the assessment of different acid digestion procedures on PM sampled on quartz filters. The solutions applied were reverse aqua regia, nitric acid, and a combination of nitric acid and hydrogen peroxide. The effect of cold-plasma treatment of samples on polycarbonate filters before TXRF measurements was also investigated. Digestion with the reverse aqua regia solution provided lower blanks and higher recovery in comparison to other tested procedures. The detection limits of the elements ranged from 0.3 to 44 ng cm−2. Ca, K, Zn, and Fe showed the highest detection limits of 44, 35, 6, and 1 ng cm−2, while As and Se had the lowest of 0.3 and 0.8 ng cm−2, respectively. The method showed higher recovery for most trace metals when applied to commercially available reference materials and field samples. TXRF measurements showed good agreement with results obtained from ion chromatography measurements for elements such as Ca and K. Cold-plasma treatment did not significantly lead to an increase in the detected concentration, and the results were element specific. Baking of the quartz filters prior to sampling showed a reduction of more than 20 % of the filter blanks for elements such as V, Sr, Mn, Zn, and Sb. The methods were applied successfully on ambient particulate matter and cloud water samples collected from the Atlas Mohammed V station in Morocco and the Cape Verde Atmospheric Observatory. The obtained concentrations were within the range reported using different techniques from similar remote and background regions elsewhere, especially for elements of anthropogenic origins such as V, Pb, and Zn with concentrations of up to 10, 19, and 28 ng m−3, respectively. Enrichment factor analysis indicated that crustal matter dominated the abundance of most of the elements, while anthropogenic activities also contributed to the abundance of elements such as Sb, Se, and Pb. The results confirm that TXRF is a useful complementary sensitive technique for trace metal analysis of particulate matter in the microgram range as well as in cloud water droplets.
A global analysis of climate-relevant aerosol properties retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
Multi-year ACSM measurements at the central European research station Melpitz (Germany)-Part 1: Instrument robustness, quality assurance, and impact of upper size cutoff diameter
The aerosol chemical speciation monitor (ACSM) is nowadays widely used to identify and quantify the main components of fine particles in ambient air. As such, its deployment at observatory platforms is fully incorporated within the European Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS). Regular intercomparisons are organized at the Aerosol Chemical Monitoring Calibration Center (ACMCC; part of the European Center for Aerosol Calibration, Paris, France) to ensure the consistency of the dataset, as well as instrumental performance and variability. However, in situ quality assurance remains a fundamental aspect of the instrument's stability. Here, we present and discuss the main outputs of long-term quality assurance efforts achieved for ACSM measurements at the research station Melpitz (Germany) since 2012 onwards. In order to validate the ACSM measurements over the years and to characterize seasonal variations, nitrate, sulfate, ammonium, organic, and particle mass concentrations were systematically compared against the collocated measurements of daily offline high-volume PM1 and PM2:5 filter samples and particle number size distribution (PNSD) measurements. Mass closure analysis was made by comparing the total particle mass (PM) concentration obtained by adding the mass concentration of equivalent black carbon (eBC) from the multi-angle absorption photometer (MAAP) to the ACSM chemical composition, to that of PM1 and PM2:5 during filter weighing, as well as to the derived mass concentration of PNSD. A combination of PM1 and PM2:5 filter samples helped identifying the critical importance of the upper size cutoff of the ACSM during such exercises. The ACSM-MAAP-derived mass concentrations systematically deviated from the PM1 mass when the mass concentration of the latter represented less than 60% of PM2:5, which was linked to the transmission efficiency of the aerodynamic lenses of the ACSM. The best correlations are obtained for sulfate (slopeD 0:96; R2 D 0:77) and total PM (slopeD 1:02; R2 D 0:90). Although, sulfate did not exhibit a seasonal dependency, total PM mass concentration revealed a small seasonal variability linked to the increase in non-water-soluble fractions. The nitrate suffers from a loss of ammonium nitrate during filter collection, and the contribution of organo-nitrate compounds to the ACSM nitrate signal make it difficult to directly compare the two methods. The contribution of m=z 44 (f44) to the total organic mass concentration was used to convert the ACSM organic mass (OM) to organic carbon (OC) by using a similar approach as for the aerosol mass spectrometer (AMS). The resulting estimated OCACSM was compared with the measured OCPM1 (slopeD 0:74; R2 D 0:77), indicating that the f44 signal was relatively free of interferences during this period. The PM2:5 filter samples use for the ACSM data quality might suffer from a systematic bias due to a size truncation effect as well as to the presence of chemical species that cannot be detected by the ACSM in coarse mode (e.g., sodium nitrate and sodium sulfate). This may lead to a systematic underestimation of the ACSM particle mass concentration and/or a positive artifact that artificially decreases the discrepancies between the two methods. Consequently, ACSM data validation using PM2:5 filters has to be interpreted with extreme care. The particle mass closure with the PNSD was satisfying (slopeD 0:77; R2 D 0:90 over the entire period), with a slight overestimation of the mobility particle size spectrometer (MPSS)-derived mass concentration in winter. This seasonal variability was related to a change on the PNSD and a larger contribution of the supermicrometer particles in winter. This long-term analysis between the ACSM and other collocated instruments confirms the robustness of the ACSM and its suitability for long-term measurements. Particle mass closure with the PNSD is strongly recommended to ensure the stability of the ACSM. A near-real-time mass closure procedure within the entire ACTRIS-ACSM network certainly represents an optimal quality control and assurance of both warranting the quality assurance of the ACSM measurements as well as identifying cross-instrumental biases. © Author(s) 2020.