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- ItemThe global aerosol-climate model echam6.3-ham2.3 -Part 1: Aerosol evaluation(Göttingen : Copernicus GmbH, 2019) Tegen, I.; Neubauer, D.; Ferrachat, S.; Drian, C.S.-L.; Bey, I.; Schutgens, N.; Stier, P.; Watson-Parris, D.; Stanelle, T.; Schmidt, H.; Rast, S.; Kokkola, H.; Schultz, M.; Schroeder, S.; Daskalakis, N.; Barthel, S.; Heinold, B.; Lohmann, U.We introduce and evaluate aerosol simulations with the global aerosol-climate model ECHAM6.3-HAM2.3, which is the aerosol component of the fully coupled aerosol-chemistry-climate model ECHAM-HAMMOZ. Both the host atmospheric climate model ECHAM6.3 and the aerosol model HAM2.3 were updated from previous versions. The updated version of the HAM aerosol model contains improved parameterizations of aerosol processes such as cloud activation, as well as updated emission fields for anthropogenic aerosol species and modifications in the online computation of sea salt and mineral dust aerosol emissions. Aerosol results from nudged and free-running simulations for the 10-year period 2003 to 2012 are compared to various measurements of aerosol properties. While there are regional deviations between the model and observations, the model performs well overall in terms of aerosol optical thickness, but may underestimate coarse-mode aerosol concentrations to some extent so that the modeled particles are smaller than indicated by the observations. Sulfate aerosol measurements in the US and Europe are reproduced well by the model, while carbonaceous aerosol species are biased low. Both mineral dust and sea salt aerosol concentrations are improved compared to previous versions of ECHAM-HAM. The evaluation of the simulated aerosol distributions serves as a basis for the suitability of the model for simulating aerosol-climate interactions in a changing climate.
- ItemDust mass, cloud condensation nuclei, and ice-nucleating particle profiling with polarization lidar: Updated POLIPHON conversion factors from global AERONET analysis(Göttingen : Copernicus GmbH, 2019) Ansmann, A.; Mamouri, R.-E.; Hofer, J.; Baars, H.; Althausen, D.; Abdullaev, S.F.The POLIPHON (Polarization Lidar Photometer Networking) method permits the retrieval of particle number, surface area, and volume concentration for dust and non-dust aerosol components. The obtained microphysical properties are used to estimate height profiles of particle mass, cloud condensation nucleus (CCN) and ice-nucleating particle (INP) concentrations. The conversion of aerosol-type-dependent particle extinction coefficients, derived from polarization lidar observations, into the aerosol microphysical properties (number, surface area, volume) forms the central part of the POLIPHON computations. The conversion parameters are determined from Aerosol Robotic Network (AERONET) aerosol climatologies of optical and microphysical properties. In this article, we focus on the dust-related POLIPHON retrieval products and present an extended set of dust conversion factors considering all relevant deserts around the globe. We apply the new conversion factor set to a dust measurement with polarization lidar in Dushanbe, Tajikistan, in central Asia. Strong aerosol layering was observed with mineral dust advected from Kazakhstan (0-2km height), Iran (2-5km), the Arabian peninsula (5-7km), and the Sahara (8-10km). POLIPHON results obtained with different sets of conversion parameters were contrasted in this central Asian case study and permitted an estimation of the conversion uncertainties.
- ItemPeakTree: A framework for structure-preserving radar Doppler spectra analysis(Göttingen : Copernicus GmbH, 2019) Radenz, M.; Bühl, J.; Seifert, P.; Griesche, H.; Engelmann, R.Clouds are frequently composed of more than one particle population even at the smallest scales. Cloud radar observations frequently contain information on multiple particle species in the observation volume when there are distinct peaks in the Doppler spectrum. Multi-peaked situations are not taken into account by established algorithms, which only use moments of the Doppler spectrum. In this study, we propose a new algorithm that recursively represents the subpeaks as nodes in a binary tree. Using this tree data structure to represent the peaks of a Doppler spectrum, it is possible to drop all a priori assumptions on the number and arrangement of subpeaks. The approach is rigid, unambiguous and can provide a basis for advanced analysis methods. The applicability is briefly demonstrated in two case studies, in which the tree structure was used to investigate particle populations in Arctic multilayered mixed-phase clouds, which were observed during the research vessel Polarstern expedition PS106 and the Atmospheric Radiation Measurement Program BAECC campaign.
- ItemMethodology for high-quality mobile measurement with focus on black carbon and particle mass concentrations(Göttingen : Copernicus GmbH, 2019) Alas, H.D.C.; Weinhold, K.; Costabile, F.; Di Ianni, A.; Müller, T.; Pfeifer, S.; Di Liberto, L.; Turner, J.R.; Wiedensohler, A.Measurements of air pollutants such as black carbon (BC) and particle mass concentration in general, using mobile platforms equipped with high-time-resolution instruments, have gained popularity over the last decade due to their wide range of applicability. Assuring the quality of mobile measurement, data have become more essential, particularly when the personal exposure to pollutants is related to their spatial distribution. In the following, we suggest a methodology to achieve data from mobile measurements of equivalent black carbon (eBC) and PM2:5 mass concentrations with high data quality. Besides frequent routine quality assurance measures of the instruments, the methodology includes the following steps: (a) measures to ensure the quality of mobile instruments through repeated collocated measurements using identical instrumentation, (b) inclusion of a fixed station along the route containing quality-assured reference instruments, and (c) sufficiently long and frequent intercomparisons between the mobile and reference instruments to correct the particle number and mass size distributions obtained from mobile measurements. The application of the methodology can provide the following results. First, collocated mobile measurements with sets of identical instruments allow identification of undetected malfunctions of the instruments. Second, frequent intercomparisons against the reference instruments will ensure the quality of the mobile measurement data of the eBC mass concentration. Third, the intercomparison data between the mobile optical particle size spectrometer (OPSS) and a reference mobility particle size spectrometer (MPSS) allow for the adjustment of the OPSS particle number size distribution using physically meaningful corrections. Matching the OPSS and MPSS volume particle size distributions is crucial for the determination of PM2:5 mass concentration. Using size-resolved complex refractive indices and time-resolved fine-mode volume correction factors of the fine-particle range, the calculated PM2:5 from the OPSS was within 5 % of the reference instruments (MPSSCAPSS). However, due to the nonsphericity and an unknown imaginary part of the complex refractive index of supermicrometer particles, a conversion to a volume equivalent diameter yields high uncertainties of the particle mass concentration greater than PM2:5. The proposed methodology addresses issues regarding the quality of mobile measurements, especially for health impact studies, validation of modeled spatial distribution, and development of air pollution mitigation strategies.
- ItemThe new BELUGA setup for collocated turbulence and radiation measurements using a tethered balloon: First applications in the cloudy Arctic boundary layer(Göttingen : Copernicus GmbH, 2019) Egerer, U.; Gottschalk, M.; Siebert, H.; Ehrlich, A.; Wendisch, M.The new BELUGA (Balloon-bornE moduLar Utility for profilinG the lower Atmosphere) tethered balloon system is introduced. It combines a set of instruments to measure turbulent and radiative parameters and energy fluxes. BELUGA enables collocated measurements either at a constant altitude or as vertical profiles up to 1.5km in height. In particular, the instrument payload of BELUGA comprises three modular instrument packages for high-resolution meteorological, wind vector and broadband radiation measurements. Collocated data acquisition allows for estimates of the driving parameters in the energy balance at various heights. Heating rates and net irradiances can be related to turbulent fluxes and local turbulence parameters such as dissipation rates. In this paper the technical setup, the instrument performance, and the measurement strategy of BELUGA are explained. Furthermore, the high vertical resolution due to the slow ascent speed is highlighted as a major advantage of tethered balloon-borne observations. Three illustrative case studies of the first application of BELUGA in the Arctic atmospheric boundary layer are presented. As a first example, measurements of a single-layer stratocumulus are discussed. They show a pronounced cloud top radiative cooling of up to 6K h-1. To put this into context, a second case elaborates respective measurements with BELUGA in a cloudless situation. In a third example, a multilayer stratocumulus was probed, revealing reduced turbulence and negligible cloud top radiative cooling for the lower cloud layer. In all three cases the net radiative fluxes are much higher than turbulent fluxes. Altogether, BELUGA has proven its robust performance in cloudy conditions of the Arctic atmospheric boundary layer.
- ItemAnnual variability of ice-nucleating particle concentrations at different Arctic locations(Göttingen : Copernicus GmbH, 2019) Wex, H.; Huang, L.; Zhang, W.; Hung, H.; Traversi, R.; Becagli, S.; Sheesley, R.J.; Moffett, C.E.; Barrett, T.E.; Bossi, R.; Skov, H.; Hünerbein, A.; Lubitz, J.; Löffler, M.; Linke, O.; Hartmann, M.; Herenz, P.; Stratmann, F.Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiagvik, formerly known as Barrow (Alaska), Nyalesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Alesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to-5 °C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs.
- ItemCoal fly ash: Linking immersion freezing behavior and physicochemical particle properties(Göttingen : Copernicus GmbH, 2018) Grawe, S.; Augustin-Bauditz, S.; Clemen, H.-C.; Ebert, M.; Eriksen Hammer, S.; Lubitz, J.; Reicher, N.; Rudich, Y.; Schneider, J.; Staacke, R.; Stratmann, F.; Welti, A.; Wex, H.To date, only a few studies have investigated the potential of coal fly ash particles to trigger heterogeneous ice nucleation in cloud droplets. The presented measurements aim at expanding the sparse dataset and improving process understanding of how physicochemical particle properties can influence the freezing behavior of coal fly ash particles immersed in water. Firstly, immersion freezing measurements were performed with two single particle techniques, i.e., the Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the SPectrometer for Ice Nuclei (SPIN). The effect of suspension time on the efficiency of the coal fly ash particles when immersed in a cloud droplet is analyzed based on the different residence times of the two instruments and employing both dry and wet particle generation. Secondly, two cold-stage setups, one using microliter sized droplets (Leipzig Ice Nucleation Array) and one using nanoliter sized droplets (WeIzmann Supercooled Droplets Observation on Microarray setup) were applied. We found that coal fly ash particles are comparable to mineral dust in their immersion freezing behavior when being dry generated. However, a significant decrease in immersion freezing efficiency was observed during experiments with wet-generated particles in LACIS and SPIN. The efficiency of wet-generated particles is in agreement with the cold-stage measurements. In order to understand the reason behind the deactivation, a series of chemical composition, morphology, and crystallography analyses (single particle mass spectrometry, scanning electron microscopy coupled with energy dispersive X-ray microanalysis, X-ray diffraction analysis) were performed with dry- and wet-generated particles. From these investigations, we conclude that anhydrous CaSO4 and CaO - which, if investigated in pure form, show the same qualitative immersion freezing behavior as observed for dry-generated coal fly ash particles - contribute to triggering heterogeneous ice nucleation at the particle-water interface. The observed deactivation in contact with water is related to changes in the particle surface properties which are potentially caused by hydration of CaSO4 and CaO. The contribution of coal fly ash to the ambient population of ice-nucleating particles therefore depends on whether and for how long particles are immersed in cloud droplets.
- ItemWildfires as a source of airborne mineral dust - Revisiting a conceptual model using large-eddy simulation (LES)(Göttingen : Copernicus GmbH, 2018) Wagner, R.; Jähn, M.; Schepanski, K.Airborne mineral dust is a key player in the Earth system and shows manifold impacts on atmospheric properties such as the radiation budget and cloud microphysics. Investigations of smoke plumes originating from wildfires found significant fractions of mineral dust within these plumes - most likely raised by strong, turbulent fire-related winds. This study presents and revisits a conceptual model describing the emission of mineral dust particles during wildfires. This is achieved by means of high-resolution large-eddy simulation (LES), conducted with the All Scale Atmospheric Model (ASAM). The impact of (a) different fire properties representing idealized grassland and shrubland fires, (b) different ambient wind conditions modulated by the fire's energy flux, and (c) the wind's capability to mobilize mineral dust particles was investigated. Results from this study illustrate that the energy release of the fire leads to a significant increase in near-surface wind speed, which consequently enhances the dust uplift potential. This is in particular the case within the fire area where vegetation can be assumed to be widely removed and uncovered soil is prone to wind erosion. The dust uplift potential is very sensitive to fire properties, such as fire size, shape, and intensity, but also depends on the ambient wind velocity. Although measurements already showed the importance of wildfires for dust emissions, pyro-convection is so far neglected as a dust emission process in atmosphere-aerosol models. The results presented in this study can be seen as the first step towards a systematic parameterization representing the connection between typical fire properties and related dust emissions.
- ItemShip-borne aerosol profiling with lidar over the Atlantic Ocean: From pure marine conditions to complex dust-smoke mixtures(Göttingen : Copernicus GmbH, 2018) Bohlmann, S.; Baars, H.; Radenz, M.; Engelmann, R.; Macke, A.The multi-wavelength Raman lidar PollyXT has been regularly operated aboard the research vessel Polarstern on expeditions across the Atlantic Ocean from north to south and vice versa. The lidar measurements of the RV Polarstern cruises PS95 from Bremerhaven, Germany, to Cape Town, Republic of South Africa (November 2015), and PS98 from Punta Arenas, Chile, to Bremerhaven, Germany (April/May 2016), are presented and analysed in detail. The latest set-up of PollyXT allows improved coverage of the marine boundary layer (MBL) due to an additional near-range receiver. Three case studies provide an overview of the aerosol detected over the Atlantic Ocean. In the first case, marine conditions were observed near South Africa on the autumn cruise PS95. Values of optical properties (depolarisation ratios close to zero, lidar ratios of 23 sr at 355 and 532 nm) within the MBL indicate pure marine aerosol. A layer of dried marine aerosol, indicated by an increase of the particle depolarisation ratio to about 10% at 355 nm (9% at 532 nm) and thus confirming the non-sphericity of these particles, could be detected on top of the MBL. On the same cruise, an almost pure Saharan dust plume was observed near the Canary Islands, presented in the second case. The third case deals with several layers of Saharan dust partly mixed with biomass-burning smoke measured on PS98 near the Cabo Verde islands. While the MBL was partly mixed with dust in the pure Saharan dust case, an almost marine MBL was observed in the third case. A statistical analysis showed latitudinal differences in the optical properties within the MBL, caused by the downmixing of dust in the tropics and anthropogenic influences in the northern latitudes, whereas the optical properties of the MBL in the Southern Hemisphere correlate with typical marine values. The particle depolarisation ratio of dried marine layers ranged between 4 and 9% at 532 nm. Night measurements from PS95 and PS98 were used to illustrate the potential of aerosol classification using lidar ratio, particle depolarisation ratio at 355 and 532 nm, and Angström exponent. Lidar ratio and particle depolarisation ratio have been found to be the main indicator for particle type, whereas the Ångström exponent is rather variable.
- ItemDepolarization and lidar ratios at 355, 532, and 1064 nm and microphysical properties of aged tropospheric and stratospheric Canadian wildfire smoke(Göttingen : Copernicus GmbH, 2018) Haarig, M.; Ansmann, A.; Baars, H.; Jimenez, C.; Veselovskii, I.; Engelmann, R.; Althausen, D.We present spectrally resolved optical and microphysical properties of western Canadian wildfire smoke observed in a tropospheric layer from 5-6.5 km height and in a stratospheric layer from 15-16 km height during a recordbreaking smoke event on 22 August 2017. Three polarization/ Raman lidars were run at the European Aerosol Research Lidar Network (EARLINET) station of Leipzig, Germany, after sunset on 22 August. For the first time, the linear depolarization ratio and extinction-to-backscatter ratio (lidar ratio) of aged smoke particles were measured at all three important lidar wavelengths of 355, 532, and 1064 nm. Very different particle depolarization ratios were found in the troposphere and in the stratosphere. The obviously compact and spherical tropospheric smoke particles caused almost no depolarization of backscattered laser radiation at all three wavelengths ( < 3 %), whereas the dry irregularly shaped soot particles in the stratosphere lead to high depolarization ratios of 22% at 355 nm and 18% at 532 nm and a comparably low value of 4% at 1064 nm. The lidar ratios were 40- 45 sr (355 nm), 65-80 sr (532 nm), and 80-95 sr (1064 nm) in both the tropospheric and stratospheric smoke layers indicating similar scattering and absorption properties. The strong wavelength dependence of the stratospheric depolarization ratio was probably caused by the absence of a particle coarse mode (particle mode consisting of particles with radius > 500nm). The stratospheric smoke particles formed a pronounced accumulation mode (in terms of particle volume or mass) centered at a particle radius of 350-400 nm. The effective particle radius was 0.32 μm. The tropospheric smoke particles were much smaller (effective radius of 0.17 μm). Mass concentrations were of the order of 5.5 μgm-3 (tropospheric layer) and 40 μgm-3 (stratospheric layer) in the night of 22 August 2017. The single scattering albedo of the stratospheric particles was estimated to be 0.74, 0.8, and 0.83 at 355, 532, and 1064 nm, respectively.