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- ItemNano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) for investigating hygroscopic properties of sub-10nm aerosol nanoparticles(Katlenburg-Lindau : Copernicus, 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, YafangInteractions 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.
- ItemProfiling water vapor mixing ratios in Finland by means of a Raman lidar, a satellite and a model(Katlenburg-Lindau : Copernicus, 2017) Filioglou, Maria; Nikandrova, Anna; Niemelä, Sami; Baars, Holger; Mielonen, Tero; Leskinen, Ari; Brus, David; Romakkaniemi, Sami; Giannakaki, Elina; Komppula, MikaWe present tropospheric water vapor profiles measured with a Raman lidar during three field campaigns held in Finland. Co-located radio soundings are available throughout the period for the calibration of the lidar signals. We investigate the possibility of calibrating the lidar water vapor profiles in the absence of co-existing on-site soundings using water vapor profiles from the combined Advanced InfraRed Sounder (AIRS) and the Advanced Microwave Sounding Unit (AMSU) satellite product; the Aire Limitée Adaptation dynamique Développement INternational and High Resolution Limited Area Model (ALADIN/HIRLAM) numerical weather prediction (NWP) system, and the nearest radio sounding station located 100 km away from the lidar site (only for the permanent location of the lidar). The uncertainties of the calibration factor derived from the soundings, the satellite and the model data are < 2.8, 7.4 and 3.9 %, respectively. We also include water vapor mixing ratio intercomparisons between the radio soundings and the various instruments/model for the period of the campaigns. A good agreement is observed for all comparisons with relative errors that do not exceed 50 % up to 8 km altitude in most cases. A 4-year seasonal analysis of vertical water vapor is also presented for the Kuopio site in Finland. During winter months, the air in Kuopio is dry (1.15±0.40 †kg-1); during summer it is wet (5.54±1.02 †kg-1); and at other times, the air is in an intermediate state. These are averaged values over the lowest 2 km in the atmosphere. Above that height a quick decrease in water vapor mixing ratios is observed, except during summer months where favorable atmospheric conditions enable higher mixing ratio values at higher altitudes. Lastly, the seasonal change in disagreement between the lidar and the model has been studied. The analysis showed that, on average, the model underestimates water vapor mixing ratios at high altitudes during spring and summer.
- ItemPolarization lidar: An extended three-signal calibration approach(Katlenburg-Lindau : Copernicus, 2019) Jimenez, Cristofer; Ansmann, Albert; Engelmann, Ronny; Haarig, Moritz; Schmidt, Jörg; Wandinger, UllaWe 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.
- ItemThe 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, JakeThe 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.
- ItemAlgorithms and uncertainties for the determination of multispectral irradiance components and aerosol optical depth from a shipborne rotating shadowband radiometer(Katlenburg-Lindau : Copernicus, 2017) Witthuhn, Jonas; Deneke, Hartwig; Macke, Andreas; Bernhard, GermarThe 19-channel rotating shadowband radiometer GUVis-3511 built by Biospherical Instruments provides automated shipborne measurements of the direct, diffuse and global spectral irradiance components without a requirement for platform stabilization. Several direct sun products, including spectral direct beam transmittance, aerosol optical depth, Ångström exponent and precipitable water, can be derived from these observations. The individual steps of the data analysis are described, and the different sources of uncertainty are discussed. The total uncertainty of the observed direct beam transmittances is estimated to be about 4% for most channels within a 95% confidence interval for shipborne operation. The calibration is identified as the dominating contribution to the total uncertainty. A comparison of direct beam transmittance with those obtained from a Cimel sunphotometer at a land site and a manually operated Microtops II sunphotometer on a ship is presented. Measurements deviate by less than 3 and 4% on land and on ship, respectively, for most channels and in agreement with our previous uncertainty estimate. These numbers demonstrate that the instrument is well suited for shipborne operation, and the applied methods for motion correction work accurately. Based on spectral direct beam transmittance, aerosol optical depth can be retrieved with an uncertainty of 0.02 for all channels within a 95% confidence interval. The different methods to account for Rayleigh scattering and gas absorption in our scheme and in the Aerosol Robotic Network processing for Cimel sunphotometers lead to minor deviations. Relying on the cross calibration of the 940 nm water vapor channel with the Cimel sunphotometer, the column amount of precipitable water can be estimated with an uncertainty of ±0.034 cm.
- ItemExperimental 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.
- ItemCloud-Aerosol Transport System (CATS) 1064 nm calibration and validation(Katlenburg-Lindau : Copernicus, 2019) Pauly, Rebecca M.; Yorks, John E.; Hlavka, Dennis L.; McGill, Matthew J.; Amiridis, Vassilis; Palm, Stephen P.; Rodier, Sharon D.; Vaughan, Mark A.; Selmer, Patrick A.; Kupchock, Andrew W.; Baars, Holger; Gialitaki, AnnaThe Cloud-Aerosol Transport System (CATS) lidar on board the International Space Station (ISS) operated from 10 February 2015 to 30 October 2017 providing range-resolved vertical backscatter profiles of Earth's atmosphere at 1064 and 532 nm. The CATS instrument design and ISS orbit lead to a higher 1064 nm signal-to-noise ratio than previous space-based lidars, allowing for direct atmospheric calibration of the 1064 nm signals. Nighttime CATS version 3-00 data were calibrated by scaling the measured data to a model of the expected atmospheric backscatter between 22 and 26 km a.m.s.l. (above mean sea level). The CATS atmospheric model is constructed using molecular backscatter profiles derived from Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) reanalysis data and aerosol scattering ratios measured by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP). The nighttime normalization altitude region was chosen to simultaneously minimize aerosol loading and variability within the CATS data frame, which extends from 28 to −2 km a.m.s.l. Daytime CATS version 3-00 data were calibrated through comparisons with nighttime measurements of the layer-integrated attenuated total backscatter (iATB) from strongly scattering, rapidly attenuating opaque cirrus clouds. The CATS nighttime 1064 nm attenuated total backscatter (ATB) uncertainties for clouds and aerosols are primarily related to the uncertainties in the CATS nighttime calibration technique, which are estimated to be ∼9  %. Median CATS V3-00 1064 nm ATB relative uncertainty at night within cloud and aerosol layers is 7 %, slightly lower than these calibration uncertainty estimates. CATS median daytime 1064 nm ATB relative uncertainty is 21 % in cloud and aerosol layers, similar to the estimated 16 %–18 % uncertainty in the CATS daytime cirrus cloud calibration transfer technique. Coincident daytime comparisons between CATS and the Cloud Physics Lidar (CPL) during the CATS-CALIPSO Airborne Validation Experiment (CCAVE) project show good agreement in mean ATB profiles for clear-air regions. Eight nighttime comparisons between CATS and the PollyXT ground-based lidars also show good agreement in clear-air regions between 3 and 12 km, with CATS having a mean ATB of 19.7 % lower than PollyXT. Agreement between the two instruments (∼7 %) is even better within an aerosol layer. Six-month comparisons of nighttime ATB values between CATS and CALIOP also show that iATB comparisons of opaque cirrus clouds agree to within 19 %. Overall, CATS has demonstrated that direct calibration of the 1064 nm channel is possible from a space-based lidar using the atmospheric normalization technique.