2020, Lei, Ting, Ma, Nan, Hong, Juan, Tuch, Thomas, Wang, Xin, Wang, Zhibin, Pöhlker, Mira, Ge, Maofa, Wang, Weigang, Mikhailov, Eugene, Hoffmann, Thorsten, Pöschl, Ulrich, Su, Hang, Wiedensohler, Alfred, Cheng, Yafang

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.

2020, Clemen, Hans-Christian, Schneider, Johannes, Klimach, Thomas, Helleis, Frank, Köllner, Franziska, Hünig, Andreas, Rubach, Florian, Mertes, Stephan, Wex, Heike, Stratmann, Frank, Welti, André, Kohl, Rebecca, Frank, Fabian, Borrmann, Stephan

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.

2020, Griessbach, Sabine, Hoffmann, Lars, Spang, Reinhold, Achtert, Peggy, von Hobe, Marc, Mateshvili, Nina, Müller, Rolf, Riese, Martin, Rolf, Christian, Seifert, Patric, Vernier, Jean-Paul

Infrared limb emission instruments have a long history in measuring clouds and aerosol. In particular, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument aboard ESA's Envisat provides 10 years of altitude-resolved global measurements. Previous studies found systematic overestimations and underestimations of cloud top heights for cirrus and polar stratospheric clouds. To assess the cloud top height information and to characterise its uncertainty for the MIPAS instrument we performed simulations for ice clouds, volcanic ash, and sulfate aerosol. From the simulation results we found that in addition to the known effects of the field-of-view that can lead to a cloud top height overestimation, and broken cloud conditions that can lead to underestimation, the cloud extinction also plays an important role. While for optically thick clouds the possible cloud top height overestimation for MIPAS reaches up to 1.6 km due to the field-of-view, for optically thin clouds and aerosol the systematic underestimation reaches 5.1 km. For the detection sensitivity and the degree of underestimation of the MIPAS measurements, the cloud layer thickness also plays a role; 1 km thick clouds are detectable down to extinctions of 5×10-4 km-1 and 6 km thick clouds are detectable down to extinctions of 1×10-4 km-1, where the largest underestimations of the cloud top height occur for the optically thinnest clouds with a vertical extent of 6 km. The relation between extinction coefficient, cloud top height estimate, and layer thickness is confirmed by a comparison of MIPAS cloud top heights of the volcanic sulfate aerosol from the Nabro eruption in 2011 with space-and ground-based lidar measurements and twilight measurements between June 2011 and February 2012. For plumes up to 2 months old, where the extinction was between 1×10-4 and 7×10-4 km-1 and the layer thickness mostly below 4 km, we found for MIPAS an average underestimation of 1.1 km. In the aged plume with extinctions down to 5 × 10-5 km-1 and layer thicknesses of up to 9.5 km, the underestimation was higher, reaching up to 7.2 km. The dependency of the cloud top height overestimations or underestimations on the extinction coefficient can explain seemingly contradictory results of previous studies. In spite of the relatively large uncertainty range of the cloud top height, the comparison of the detection sensitivity towards sulfate aerosol between MIPAS and a suite of widely used UV/VIS limb and IR nadir satellite aerosol measurements shows that MIPAS provides complementary information in terms of detection sensitivity. © Author(s) 2020.

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).

2020, Griesche, Hannes J., Seifer, Patric, Ansmann, Albert, Baars, Holger, Velasco, Carola Barrientos, Bühl, Johannes, Engelmann, Ronny, Radenz, Martin, Zhenping, Yin, Macke, Andreas

From 25 May to 21 July 2017, the research vessel Polarstern performed the cruise PS106 to the high Arctic in the region north and northeast of Svalbard. The mobile remote-sensing platform OCEANET was deployed aboard Polarstern. Within a single container, OCEANET houses state-of-the-art remote-sensing equipment, including a multiwavelength Raman polarization lidar PollyXT and a 14-channel microwave radiometer HATPRO (Humidity And Temperature PROfiler). For the cruise PS106, the measurements were supplemented by a motion-stabilized 35 GHz cloud radar Mira-35. This paper describes the treatment of technical challenges which were immanent during the deployment of OCEANET in the high Arctic. This includes the description of the motion stabilization of the cloud radar Mira-35 to ensure vertical-pointing observations aboard the moving Polarstern as well as the applied correction of the vessels heave rate to provide valid Doppler velocities. The correction ensured a leveling accuracy of ±0.5◦ during transits through the ice and an ice floe camp. The applied heave correction reduced the signal induced by the vertical movement of the cloud radar in the PSD of the Doppler velocity by a factor of 15. Low-level clouds, in addition, frequently prevented a continuous analysis of cloud conditions from synergies of lidar and radar within Cloudnet, because the technically determined lowest detection height of Mira-35 was 165 m above sea level. To overcome this obstacle, an approach for identification of the cloud presence solely based on data from the near-field receiver of PollyXT at heights from 50 m and 165 m above sea level is presented. We found low-level stratus clouds, which were below the lowest detection range of most automatic ground-based remote-sensing instruments during 25 % of the observation time. We present case studies of aerosol and cloud studies to introduce the capabilities of the data set. In addition, new approaches for ice crystal effective radius and eddy dissipation rates from cloud radar measurements and the retrieval of aerosol optical and microphysical properties from the observations of PollyXT are introduced. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.

2020, Giannakaki, Elina, Kokkalis, Panos, Marinou, Eleni, Bartsotas, Nikolaos S., Amiridis, Vassilis, Ansmann, Albert, Komppula, Mika

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).

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.