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Start date: 2020 × End date: 2019 × Start date: 2018 × Has files: Yes × Publisher: Katlenburg-Lindau : Copernicus × Subject: measurement method × WGL Institute: TROPOS ×

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    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)?
    (Katlenburg-Lindau : Copernicus, 2019) Tesche, Matthias; Kolgotin, Alexei; Haarig, Moritz; Burton, Sharon P.; Ferrare, Richard A.; Hostetler, Chris A.; Müller, Detlef
    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).
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    Separation of the optical and mass features of particle components in different aerosol mixtures by using POLIPHON retrievals in synergy with continuous polarized Micro-Pulse Lidar (P-MPL) measurements
    (Katlenburg-Lindau : Copernicus, 2018) Córdoba-Jabonero, Carmen; Sicard, Michaël; Ansmann, Albert; del Águila, Ana; Baars, Holger
    The application of the POLIPHON (POlarization-LIdar PHOtometer Networking) method is presented for the first time in synergy with continuous 24/7 polarized Micro-Pulse Lidar (P-MPL) measurements to derive the vertical separation of two or three particle components in different aerosol mixtures, and the retrieval of their particular optical properties. The procedure of extinction-to-mass conversion, together with an analysis of the mass extinction efficiency (MEE) parameter, is described, and the relative mass contribution of each aerosol component is also derived in a further step. The general POLIPHON algorithm is based on the specific particle linear depolarization ratio given for different types of aerosols and can be run in either 1-step (POL-1) or 2 steps (POL-2) versions with dependence on either the 2- or 3-component separation. In order to illustrate this procedure, aerosol mixing cases observed over Barcelona (NE Spain) are selected: a dust event on 5 July 2016, smoke plumes detected on 23 May 2016 and a pollination episode observed on 23 March 2016. In particular, the 3-component separation is just applied for the dust case: a combined POL-1 with POL-2 procedure (POL-1/2) is used, and additionally the fine-dust contribution to the total fine mode (fine dust plus non-dust aerosols) is estimated. The high dust impact before 12:00 UTC yields a mean mass loading of 0.6±0.1 g m'2 due to the prevalence of Saharan coarse-dust particles. After that time, the mean mass loading is reduced by two-thirds, showing a rather weak dust incidence. In the smoke case, the arrival of fine biomass-burning particles is detected at altitudes as high as 7 km. The smoke particles, probably mixed with less depolarizing non-smoke aerosols, are observed in air masses, having their origin from either North American fires or the Arctic area, as reported by HYSPLIT back-trajectory analysis. The particle linear depolarization ratio for smoke shows values in the 0.10-0.15 range and even higher at given times, and the daily mean smoke mass loading is 0.017±0.008 g m'2, around 3 % of that found for the dust event. Pollen particles are detected up to 1.5 km in height from 10:00 UTC during an intense pollination event with a particle linear depolarization ratio ranging between 0.10 and 0.15. The maximal mass loading of Platanus pollen particles is 0.011±0.003 g m'2, representing around 2 % of the dust loading during the higher dust incidence. Regarding the MEE derived for each aerosol component, their values are in agreement with others referenced in the literature for the specific aerosol types examined in this work: 0.5±0.1 and 1.7±0.2 m2 g'1 are found for coarse and fine dust particles, 4.5±1.4 m2 g'1 is derived for smoke and 2.4±0.5 m2 g'1 for non-smoke aerosols with Arctic origin, and a MEE of 2.4±0.8 m2 g'1 is obtained for pollen particles, though it can reach higher or lower values depending on predominantly smaller or larger pollen grain sizes. Results reveal the high potential of the P-MPL system, a simple polarization-sensitive elastic backscatter lidar working in a 24/7 operation mode, to retrieve the relative optical and mass contributions of each aerosol component throughout the day, reflecting the daily variability of their properties. In fact, this procedure can be simply implemented in other P-MPLs that also operate within the worldwide Micro-Pulse Lidar Network (MPLNET), thus extending the aerosol discrimination at a global scale. Moreover, the method has the advantage of also being relatively easily applicable to space-borne lidars with an equivalent configuration such as the ongoing Cloud-Aerosol LIdar with Orthogonal Polarization (CALIOP) on board NASA CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) and the forthcoming Atmospheric Lidar (ATLID) on board the ESA EarthCARE mission.
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    The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): Laboratory intercomparison of ice nucleation measurements
    (Katlenburg-Lindau : Copernicus, 2018) DeMott, Paul J.; Möhler, Ottmar; Cziczo, Daniel J.; Hiranuma, Naruki; Petters, Markus D.; Petters, Sarah S.; Belosi, Franco; Bingemer, Heinz G.; Brooks, Sarah D.; Budke, Carsten; Burkert-Kohn, Monika; Collier, Kristen N.; Danielczok, Anja; Eppers, Oliver; Felgitsch, Laura; Garimella, Sarvesh; Grothe, Hinrich; Herenz, Paul; Hill, Thomas C. J.; Höhler, Kristina; Kanji, Zamin A.; Kiselev, Alexei; Koop, Thomas; Kristensen, Thomas B.; Krüger, Konstantin; Kulkarni, Gourihar; Levin, Ezra J. T.; Murray, Benjamin J.; Nicosia, Alessia; O'Sullivan, Daniel; Peckhaus, Andreas; Polen, Michael J.; Price, Hannah C.; Reicher, Naama; Rothenberg, Daniel A.; Rudich, Yinon; Santachiara, Gianni; Schiebel, Thea; Schrod, Jann; Seifried, Teresa M.; Stratmann, Frank; Sullivan, Ryan C.; Suski, Kaitlyn J.; Szakáll, Miklós; Taylor, Hans P.; Ullrich, Romy; Vergara-Temprado, Jesus; Wagner, Robert; Whale, Thomas F.; Weber, Daniel; Welti, André; Wilson, Theodore W.; Wolf, Martin J.; Zenker, Jake
    The second phase of the Fifth International Ice Nucleation Workshop (FIN-02) involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere (AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide. Compared to the previous workshop in 2007, participation was doubled, reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques that post-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing. The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam (Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively, and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good in most cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber-Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this is not always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than -10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling for K-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with parameterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illite NX by direct versus post-processing methods were not repeated for other particle types, and the Snomax° data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.
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    Experimental techniques for the calibration of lidar depolarization channels in EARLINET
    (Katlenburg-Lindau : Copernicus, 2018) Belegante, Livio; Bravo-Aranda, Juan Antonio; Freudenthaler, Volker; Nicolae, Doina; Nemuc, Anca; Ene, Dragos; Alados-Arboledas, Lucas; Amodeo, Aldo; Pappalardo, Gelsomina; D'Amico, Giuseppe; Amato, Francesco; Engelmann, Ronny; Baars, Holger; Wandinger, Ulla; Papayannis, Alexandros; Kokkalis, Panos; Pereira, Sérgio N.
    Particle depolarization ratio retrieved from lidar measurements are commonly used for aerosol-typing studies, microphysical inversion, or mass concentration retrievals. The particle depolarization ratio is one of the primary parameters that can differentiate several major aerosol components but only if the measurements are accurate enough. The accuracy related to the retrieval of particle depolarization ratios is the driving factor for assessing and improving the uncertainties of the depolarization products. This paper presents different depolarization calibration procedures used to improve the quality of the depolarization data. The results illustrate a significant improvement of the depolarization lidar products for all the selected lidar stations that have implemented depolarization calibration procedures. The calibrated volume and particle depolarization profiles at 532-nm show values that fall within a range that is generally accepted in the literature.
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    The effect of rapid relative humidity changes on fast filter-based aerosol-particle light-absorption measurements: Uncertainties and correction schemes
    (Katlenburg-Lindau : Copernicus, 2019) Düsing, Sebastian; Wehner, Birgit; Müller, Thomas; Stöcker, Almond; Wiedensohler, Alfred
    Measuring vertical profiles of the particle light-absorption coefficient by using absorption photometers may face the challenge of fast changes in relative humidity (RH). These absorption photometers determine the particle light-absorption coefficient due to a change in light attenuation through a particle-loaded filter. The filter material, however, takes up or releases water with changing relative humidity (RH in %), thus influencing the light attenuation. A sophisticated set of laboratory experiments was therefore conducted to investigate the effect of fast RH changes (dRH/dt) on the particle light-absorption coefficient (σabs in Mm-1) derived with two absorption photometers. The RH dependence was examined based on different filter types and filter loadings with respect to loading material and areal loading density. The Single Channel Tricolor Absorption Photometer (STAP) relies on quartz-fiber filter, and the microAeth® MA200 is based on a polytetrafluoroethylene (PTFE) filter band. Furthermore, three cases were investigated: clean filters, filters loaded with black carbon (BC), and filters loaded with ammonium sulfate. The filter areal loading densities (ρ∗) ranged from 3.1 to 99.6 mg m-2 in the case of the STAP and ammonium sulfate and 1.2 to 37.6 mg m-2 in the case the MA200. Investigating BC-loaded cases, M8 scroll mrow miBCm 15pt was in the range of 2.9 to 43.0 and 1.1 to 16.3 mg m-2 for the STAP and MA200, respectively.

    Both instruments revealed opposing responses to relative humidity changes ("RH) with different magnitudes. The STAP shows a linear dependence on relative humidity changes. The MA200 is characterized by a distinct exponential recovery after its filter was exposed to relative humidity changes. At a wavelength of 624 nm and for the default 60 s running average output, the STAP reveals an absolute change in σabs per absolute change of RH ("σabsĝ•"RH) of 0.14 Mm-1 %-1 in the clean case, 0.29 Mm-1 %-1 in the case of BC-loaded filters, and 0.21 Mm-1 %-1 in the case filters loaded with ammonium sulfate. The 60 s running average of the particle light-absorption coefficient at 625 nm measured with the MA200 revealed a response of around -0.4 Mm-1 %-1 for all three cases. Whereas the response of the STAP varies over the different loading materials, in contrast, the MA200 was quite stable. The response was, for the STAP, in the range of 0.17 to 0.24 Mm-1 %-1 and, in the case of ammonium sulfate loading and in the BC-loaded case, 0.17 to 0.62 Mm-1 %-1. In the ammonium sulfate case, the minimum response shown by the MA200 was -0.42 with a maximum of -0.36 Mm-1 %-1 and a minimum of -0.42 and maximum -0.37 Mm-1 %-1 in the case of BC.

    A linear correction function for the STAP was developed here. It is provided by correlating 1 Hz resolved recalculated particle light-absorption coefficients and RH change rates. The linear response is estimated at 10.08 Mm-1 s-1 %-1. A correction approach for the MA200 is also provided; however, the behavior of the MA200 is more complex. Further research and multi-instrument measurements have to be conducted to fully understand the underlying processes, since the correction approach resulted in different correction parameters across various experiments. However, the exponential recovery after the filter of the MA200 experienced a RH change could be reproduced. However, the given correction approach has to be estimated with other RH sensors as well, since each sensor has a different response time. And, for the given correction approaches, the uncertainties could not be estimated, which was mainly due to the response time of the RH sensor. Therefore, we do not recommend using the given approaches. But they point in the right direction, and despite the imperfections, they are useful for at least estimating the measurement uncertainties due to relative humidity changes.

    Due to our findings, we recommend using an aerosol dryer upstream of absorption photometers to reduce the RH effect significantly. Furthermore, when absorption photometers are used in vertical measurements, the ascending or descending speed through layers of large relative humidity gradients has to be low to minimize the observed RH effect. But this is simply not possible in some scenarios, especially in unmixed layers or clouds. Additionally, recording the RH of the sample stream allows correcting for the bias during post-processing of the data. This data correction leads to reasonable results, according to the given example in this study. © Author(s) 2019.