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- ItemAcidity and the multiphase chemistry of atmospheric aqueous particles and clouds(Katlenburg-Lindau : European Geosciences Union, 2021) Tilgner, Andreas; Schaefer, Thomas; Alexander, Becky; Barth, Mary; Collett, Jeffrey L.; Fahey, Kathleen M.; Nenes, Athanasios; Pye, Havala O.T.; Herrmann, Hartmut; McNeill, V. FayeThe acidity of aqueous atmospheric solutions is a key parameter driving both the partitioning of semi-volatile acidic and basic trace gases and their aqueous-phase chemistry. In addition, the acidity of atmospheric aqueous phases, e.g., deliquesced aerosol particles, cloud, and fog droplets, is also dictated by aqueous-phase chemistry. These feedbacks between acidity and chemistry have crucial implications for the tropospheric lifetime of air pollutants, atmospheric composition, deposition to terrestrial and oceanic ecosystems, visibility, climate, and human health. Atmospheric research has made substantial progress in understanding feedbacks between acidity and multiphase chemistry during recent decades. This paper reviews the current state of knowledge on these feedbacks with a focus on aerosol and cloud systems, which involve both inorganic and organic aqueous-phase chemistry. Here, we describe the impacts of acidity on the phase partitioning of acidic and basic gases and buffering phenomena. Next, we review feedbacks of different acidity regimes on key chemical reaction mechanisms and kinetics, as well as uncertainties and chemical subsystems with incomplete information. Finally, we discuss atmospheric implications and highlight the need for future investigations, particularly with respect to reducing emissions of key acid precursors in a changing world, and the need for advancements in field and laboratory measurements and model tools.
- ItemLIVAS: A 3-D multi-wavelength aerosol/cloud database based on CALIPSO and EARLINET(München : European Geopyhsical Union, 2015) Amiridis, V.; Marinou, E.; Tsekeri, A.; Wandinger, U.; Schwarz, A.; Giannakaki, E.; Mamouri, R.; Kokkalis, P.; Binietoglou, I.; Solomos, S.; Herekakis, T.; Kazadzis, S.; Gerasopoulos, E.; Proestakis, E.; Kottas, M.; Balis, D.; Papayannis, A.; Kontoes, C.; Kourtidis, K.; Papagiannopoulos, N.; Mona, L.; Pappalardo, G.; Le Rille, O.; Ansmann, A.We present LIVAS (LIdar climatology of Vertical Aerosol Structure for space-based lidar simulation studies), a 3-D multi-wavelength global aerosol and cloud optical database, optimized to be used for future space-based lidar end-to-end simulations of realistic atmospheric scenarios as well as retrieval algorithm testing activities. The LIVAS database provides averaged profiles of aerosol optical properties for the potential spaceborne laser operating wavelengths of 355, 532, 1064, 1570 and 2050 nm and of cloud optical properties at the wavelength of 532 nm. The global database is based on CALIPSO observations at 532 and 1064 nm and on aerosol-type-dependent backscatter- and extinction-related Ångström exponents, derived from EARLINET (European Aerosol Research Lidar Network) ground-based measurements for the UV and scattering calculations for the IR wavelengths, using a combination of input data from AERONET, suitable aerosol models and recent literature. The required spectral conversions are calculated for each of the CALIPSO aerosol types and are applied to CALIPSO backscatter and extinction data corresponding to the aerosol type retrieved by the CALIPSO aerosol classification scheme. A cloud optical database based on CALIPSO measurements at 532 nm is also provided, neglecting wavelength conversion due to approximately neutral scattering behavior of clouds along the spectral range of LIVAS. Averages of particle linear depolarization ratio profiles at 532 nm are provided as well. Finally, vertical distributions for a set of selected scenes of specific atmospheric phenomena (e.g., dust outbreaks, volcanic eruptions, wild fires, polar stratospheric clouds) are analyzed and spectrally converted so as to be used as case studies for spaceborne lidar performance assessments. The final global data set includes 4-year (1 January 2008–31 December 2011) time-averaged CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) data on a uniform grid of 1° × 1° with the original high vertical resolution of CALIPSO in order to ensure realistic simulations of the atmospheric variability in lidar end-to-end simulations.
- ItemIn-cloud sulfate addition to single particles resolved with sulfur isotope analysis during HCCT-2010(München : European Geopyhsical Union, 2014) Harris, E.; Sinha, B.; van Pinxteren, D.; Schneider, J.; Poulain, L.; Collett, J.; D'Anna, B.; Fahlbusch, B.; Foley, S.; Fomba, K.W.; George, C.; Gnauk, T.; Henning, S.; Lee, T.; Mertes, S.; Roth, A.; Stratmann, F.; Borrmann, S.; Hoppe, P.; Herrmann, H.In-cloud production of sulfate modifies aerosol size distribution, with important implications for the magnitude of indirect and direct aerosol cooling and the impact of SO2 emissions on the environment. We investigate which sulfate sources dominate the in-cloud addition of sulfate to different particle classes as an air parcel passes through an orographic cloud. Sulfate aerosol, SO2 and H2SO4 were collected upwind, in-cloud and downwind of an orographic cloud for three cloud measurement events during the Hill Cap Cloud Thuringia campaign in autumn 2010 (HCCT-2010). Combined SEM and NanoSIMS analysis of single particles allowed the δ34S of particulate sulfate to be resolved for particle size and type. The most important in-cloud SO2 oxidation pathway at HCCT-2010 was aqueous oxidation catalysed by transition metal ions (TMI catalysis), which was shown with single particle isotope analyses to occur primarily in cloud droplets nucleated on coarse mineral dust. In contrast, direct uptake of H2SO4 (g) and ultrafine particulate were the most important sources modifying fine mineral dust, increasing its hygroscopicity and facilitating activation. Sulfate addition to "mixed" particles (secondary organic and inorganic aerosol) and coated soot was dominated by in-cloud aqueous SO2 oxidation by H2O2 and direct uptake of H2SO4 (g) and ultrafine particle sulfate, depending on particle size mode and time of day. These results provide new insight into in-cloud sulfate production mechanisms, and show the importance of single particle measurements and models to accurately assess the environmental effects of cloud processing.
- ItemStable water isotopologue ratios in fog and cloud droplets of liquid clouds are not size-dependent(München : European Geopyhsical Union, 2012) Spiegel, J.K.; Aemisegger, F.; Scholl, M.; Wienhold, F.G.; Collett Jr., J.L.; Lee, T.; van Pinxteren, D.; Mertes, S.; Tilgner, A.; Herrmann, H.; Werner, R.A.; Buchmann, N.; Eugster, W.In this work, we present the first observations of stable water isotopologue ratios in cloud droplets of different sizes collected simultaneously. We address the question whether the isotope ratio of droplets in a liquid cloud varies as a function of droplet size. Samples were collected from a ground intercepted cloud (= fog) during the Hill Cap Cloud Thuringia 2010 campaign (HCCT-2010) using a three-stage Caltech Active Strand Cloud water Collector (CASCC). An instrument test revealed that no artificial isotopic fractionation occurs during sample collection with the CASCC. Furthermore, we could experimentally confirm the hypothesis that the δ values of cloud droplets of the relevant droplet sizes (μm-range) were not significantly different and thus can be assumed to be in isotopic equilibrium immediately with the surrounding water vapor. However, during the dissolution period of the cloud, when the supersaturation inside the cloud decreased and the cloud began to clear, differences in isotope ratios of the different droplet sizes tended to be larger. This is likely to result from the cloud's heterogeneity, implying that larger and smaller cloud droplets have been collected at different moments in time, delivering isotope ratios from different collection times.
- ItemTarget categorization of aerosol and clouds by continuous multiwavelength-polarization lidar measurements(Katlenburg-Lindau : Copernicus, 2017) Baars, Holger; Seifert, Patric; Engelmann, Ronny; Wandinger, UllaAbsolute calibrated signals at 532 and 1064 nm and the depolarization ratio from a multiwavelength lidar are used to categorize primary aerosol but also clouds in high temporal and spatial resolution. Automatically derived particle backscatter coefficient profiles in low temporal resolution (30 min) are applied to calibrate the lidar signals. From these calibrated lidar signals, new atmospheric parameters in temporally high resolution (quasi-particle-backscatter coefficients) are derived. By using thresholds obtained from multiyear, multisite EARLINET (European Aerosol Research Lidar Network) measurements, four aerosol classes (small; large, spherical; large, non-spherical; mixed, partly nonspherical) and several cloud classes (liquid, ice) are defined. Thus, particles are classified by their physical features (shape and size) instead of by source. The methodology is applied to 2 months of continuous observations (24 h a day, 7 days a week) with the multiwavelength-Raman-polarization lidar PollyXT during the High-Definition Clouds and Precipitation for advancing Climate Prediction (HD(CP)2) Observational Prototype Experiment (HOPE) in spring 2013. Cloudnet equipment was operated continuously directly next to the lidar and is used for comparison. By discussing three 24 h case studies, it is shown that the aerosol discrimination is very feasible and informative and gives a good complement to the Cloudnet target categorization. Performing the categorization for the 2-month data set of the entire HOPE campaign, almost 1 million pixel (5 min×30 m) could be analysed with the newly developed tool. We find that the majority of the aerosol trapped in the planetary boundary layer (PBL) was composed of small particles as expected for a heavily populated and industrialized area. Large, spherical aerosol was observed mostly at the top of the PBL and close to the identified cloud bases, indicating the importance of hygroscopic growth of the particles at high relative humidity. Interestingly, it is found that on several days non-spherical particles were dispersed from the ground into the atmosphere.
- ItemSchneefernerhaus as a mountain research station for clouds and turbulence(München : European Geopyhsical Union, 2015) Risius, S.; Xu, H.; Di Lorenzo, F.; Xi, H.; Siebert, H.; Shaw, R.A.; Bodenschatz, E.Cloud measurements are usually carried out with airborne campaigns, which are expensive and are limited by temporal duration and weather conditions. Ground-based measurements at high-altitude research stations therefore play a complementary role in cloud study. Using the meteorological data (wind speed, direction, temperature, humidity, visibility, etc.) collected by the German Weather Service (DWD) from 2000 to 2012 and turbulence measurements recorded by multiple ultrasonic sensors (sampled at 10 Hz) in 2010, we show that the Umweltforschungsstation Schneefernerhaus (UFS) located just below the peak of Zugspitze in the German Alps, at a height of 2650 m, is a well-suited station for cloud–turbulence research. The wind at UFS is dominantly in the east–west direction and nearly horizontal. During the summertime (July and August) the UFS is immersed in warm clouds about 25 % of the time. The clouds are either from convection originating in the valley in the east, or associated with synoptic-scale weather systems typically advected from the west. Air turbulence, as measured from the second- and third-order velocity structure functions that exhibit well-developed inertial ranges, possesses Taylor microscale Reynolds numbers up to 104, with the most probable value at ~ 3000. In spite of the complex topography, the turbulence appears to be nearly as isotropic as many laboratory flows when evaluated on the "Lumley triangle".
- ItemA methodology for investigating dust model performance using synergistic EARLINET/AERONET dust concentration retrievals(München : European Geopyhsical Union, 2015) Binietoglou, I.; Basart, S.; Alados-Arboledas, L.; Amiridis, V.; Argyrouli, A.; Baars, H.; Baldasano, J.M.; Balis, D.; Belegante, L.; Bravo-Aranda, J.A.; Burlizzi, P.; Carrasco, V.; Chaikovsky, A.; Comerón, A.; D'Amico, G.; Filioglou, M.; Granados-Muñoz, M.J.; Haefele, A.; Hervo, M.; Iarlori, M.; Kokkalis, P.; Lange, D.; Mamouri, R.E.; Mattis, I.; Molero, F.; Montoux, N.; Muñoz, A.; Muñoz Porcar, C.; Navas-Guzmán, F.; Nicolae, D.; Nisantzi, A.; Papagiannopoulos, N.; Papayannis, A.; Pereira, S.; Preißler, J.; Pujadas, M.; Rizi, V.; Rocadenbosch, F.; Sellegri, K.; Simeonov, V.; Tsaknakis, G.; Wagner, F.; Pappalardo, G.Systematic measurements of dust concentration profiles at a continental scale were recently made possible by the development of synergistic retrieval algorithms using combined lidar and sun photometer data and the establishment of robust remote-sensing networks in the framework of Aerosols, Clouds, and Trace gases Research InfraStructure Network (ACTRIS)/European Aerosol Research Lidar Network (EARLINET). We present a methodology for using these capabilities as a tool for examining the performance of dust transport models. The methodology includes considerations for the selection of a suitable data set and appropriate metrics for the exploration of the results. The approach is demonstrated for four regional dust transport models (BSC-DREAM8b v2, NMMB/BSC-DUST, DREAMABOL, DREAM8-NMME-MACC) using dust observations performed at 10 ACTRIS/EARLINET stations. The observations, which include coincident multi-wavelength lidar and sun photometer measurements, were processed with the Lidar-Radiometer Inversion Code (LIRIC) to retrieve aerosol concentration profiles. The methodology proposed here shows advantages when compared to traditional evaluation techniques that utilize separately the available measurements such as separating the contribution of dust from other aerosol types on the lidar profiles and avoiding model assumptions related to the conversion of concentration fields to aerosol extinction values. When compared to LIRIC retrievals, the simulated dust vertical structures were found to be in good agreement for all models with correlation values between 0.5 and 0.7 in the 1–6 km range, where most dust is typically observed. The absolute dust concentration was typically underestimated with mean bias values of -40 to -20 μg m−3 at 2 km, the altitude of maximum mean concentration. The reported differences among the models found in this comparison indicate the benefit of the systematic use of the proposed approach in future dust model evaluation studies.
- ItemDevelopment and validation of a supervised machine learning radar Doppler spectra peak-finding algorithm(Katlenburg-Lindau : Copernicus, 2019) Kalesse, Heike; Vogl, Teresa; Paduraru, Cosmin; Luke, EdwardIn many types of clouds, multiple hydrometeor populations can be present at the same time and height. Studying the evolution of these different hydrometeors in a time-height perspective can give valuable information on cloud particle composition and microphysical growth processes. However, as a prerequisite, the number of different hydrometeor types in a certain cloud volume needs to be quantified. This can be accomplished using cloud radar Doppler velocity spectra from profiling cloud radars if the different hydrometeor types have sufficiently different terminal fall velocities to produce individual Doppler spectrum peaks. Here we present a newly developed supervised machine learning radar Doppler spectra peak-finding algorithm (named PEAKO). In this approach, three adjustable parameters (spectrum smoothing span, prominence threshold, and minimum peak width at half-height) are varied to obtain the set of parameters which yields the best agreement of user-classified and machine-marked peaks. The algorithm was developed for Ka-band ARM zenith-pointing radar (KAZR) observations obtained in thick snowfall systems during the Atmospheric Radiation Measurement Program (ARM) mobile facility AMF2 deployment at Hyytiälä, Finland, during the Biogenic Aerosols - Effects on Clouds and Climate (BAECC) field campaign. The performance of PEAKO is evaluated by comparing its results to existing Doppler peak-finding algorithms. The new algorithm consistently identifies Doppler spectra peaks and outperforms other algorithms by reducing noise and increasing temporal and height consistency in detected features. In the future, the PEAKO algorithm will be adapted to other cloud radars and other types of clouds consisting of multiple hydrometeors in the same cloud volume. © 2019 Copernicus GmbH. All rights reserved.
- ItemAerosol dynamics and dispersion of radioactive particles(Katlenburg-Lindau : European Geosciences Union, 2021) Schoenberg, Pontus von; Tunved, Peter; Grahn, Håkan; Wiedensohler, Alfred; Krejci, Radovan; Brännström, NiklasIn the event of a failure of a nuclear power plant with release of radioactive material into the atmosphere, dispersion modelling is used to understand how the released radioactivity is spread. For the dispersion of particles, Lagrangian particle dispersion models (LPDMs) are commonly used, in which model particles, representing the released material, are transported through the atmosphere. These model particles are usually inert and undergo only first-order processes such as dry deposition and simplified wet deposition along the path through the atmosphere. Aerosol dynamic processes including coagulation, condensational growth, chemical interactions, formation of new particles and interaction with new aerosol sources are usually neglected in such models. The objective of this study is to analyse the impact of these advanced aerosol dynamic processes if they were to be included in LPDM simulations for use in radioactive preparedness. In this investigation, a fictitious failure of a nuclear power plant is studied for three geographically and atmospherically different sites. The incident was simulated with a Lagrangian single-trajectory box model with a new simulation for each hour throughout a year to capture seasonal variability of meteorology and variation in the ambient aerosol. (a) We conclude that modelling of wet deposition by incorporating an advanced cloud parameterization is advisable, since it significantly influence simulated levels of airborne and deposited activity including radioactive hotspots, and (b) we show that inclusion of detailed ambient-aerosol dynamics can play a large role in the model result in simulations that adopt a more detailed representation of aerosol–cloud interactions. The results highlight a potential necessity for implementation of more detailed representation of general aerosol dynamic processes into LPDMs in order to cover the full range of possible environmental characteristics that can apply during a release of radionuclides into the atmosphere.
- ItemGlobal relevance of marine organic aerosol as ice nucleating particles(Katlenburg-Lindau : EGU, 2018) Huang, Wan Ting Katty; Ickes, Luisa; Tegen, Ina; Rinaldi, Matteo; Ceburnis, Darius; Lohmann, UlrikeIce nucleating particles (INPs) increase the temperature at which supercooled droplets start to freeze. They are therefore of particular interest in mixed-phase cloud temperature regimes, where supercooled liquid droplets can persist for extended periods of time in the absence of INPs. When INPs are introduced to such an environment, the cloud can quickly glaciate following ice multiplication processes and the Wegener–Bergeron–Findeisen (WBF) process. The WBF process can also cause the ice to grow to precipitation size and precipitate out. All of these processes alter the radiative properties. Despite their potential influence on climate, the ice nucleation ability and importance of different aerosol species is still not well understood and is a field of active research. In this study, we use the aerosol–climate model ECHAM6-HAM2 to examine the global relevance of marine organic aerosol (MOA), which has drawn much interest in recent years as a potentially important INPs in remote marine regions. We address the uncertainties in emissions and ice nucleation activity of MOA with a range of reasonable set-ups and find a wide range of resulting MOA burdens. The relative importance of MOA as an INP compared to dust is investigated and found to depend strongly on the type of ice nucleation parameterisation scheme chosen. On the zonal mean, freezing due to MOA leads to relative increases in the cloud ice occurrence and in-cloud number concentration close to the surface in the polar regions during summer. Slight but consistent decreases in the in-cloud ice crystal effective radius can also be observed over the same regions during all seasons. Regardless, MOA was not found to affect the radiative balance significantly on the global scale, due to its relatively weak ice activity and a low sensitivity of cloud ice properties to heterogeneous ice nucleation in our model.