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- 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.
- 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.
- ItemLarge-scale modeling of absorbing aerosols and their semi-direct effects(Basel : MDPI AG, 2018) Tegen, I.; Heinold, B.Radiative effects of absorbing black carbon and mineral dust aerosols are estimated from global aerosol climate model simulations with fixed sea surface temperatures as a boundary condition. Semi-direct effects are approximated as the residual between the total direct radiative effect and the instantaneous direct radiative effect of the simulated absorbing aerosol species. No distinction is made for aerosols from natural and anthropogenic sources. Results for global average are highly uncertain due to high model variability, but consistent with previous estimates. The global average results for black carbon aerosol semi-direct effects are small due to cancellation of regionally positive or negative effects, and may be positive or negative overall, depending on the model setup. The presence of mineral dust aerosol above dark surfaces and below a layer containing black carbon aerosol may enhance the reflectivity and act to enhance the positive radiative effect of black carbon aerosol. When mineral dust is absent the semi-direct effect at the top-of-atmosphere of black carbon aerosol from both anthropogenic and natural sources is -0.03 Wm-2, while averaging to +0.09 Wm-2 if dust is included.
- 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.
- ItemThe second ACTRIS inter-comparison (2016) for Aerosol Chemical Speciation Monitors (ACSM): Calibration protocols and instrument performance evaluations(Philadelphia, Pa.: Taylor & Francis, 2019) Freney, Evelyn; Zhang, Yunjiang; Croteau, Philip; Amodeo, Tanguy; Williams, Leah; Truong, François; Petit, Jean-Eudes; Sciare, Jean; Sarda-Esteve, Roland; Bonnaire, Nicolas; Arumae, Tarvo; Aurela, Minna; Bougiatioti, Aikaterini; Mihalopoulos, Nikolaos; Coz, Esther; Artinano, Begoña; Crenn, Vincent; Elste, Thomas; Heikkinen, Liine; Poulain, Laurent; Wiedensohler, Alfred; Herrmann, Hartmut; Priestman, Max; Alastuey, Andres; Stavroulas, Iasonas; Tobler, Anna; Vasilescu, Jeni; Zanca, Nicola; Canagaratna, Manjula; Carbone, Claudio; Flentje, Harald; Green, David; Maasikmets, Marek; Marmureanu, Luminita; Cruz Minguillon, Maria; Prevot, Andre S.H.; Gros, Valerie; Jayne, John; Favez, OlivierThis work describes results obtained from the 2016 Aerosol Chemical Speciation Monitor (ACSM) intercomparison exercise performed at the Aerosol Chemical Monitor Calibration Center (ACMCC, France). Fifteen quadrupole ACSMs (Q_ACSM) from the European Research Infrastructure for the observation of Aerosols, Clouds and Trace gases (ACTRIS) network were calibrated using a new procedure that acquires calibration data under the same operating conditions as those used during sampling and hence gets information representative of instrument performance. The new calibration procedure notably resulted in a decrease in the spread of the measured sulfate mass concentrations, improving the reproducibility of inorganic species measurements between ACSMs as well as the consistency with co-located independent instruments. Tested calibration procedures also allowed for the investigation of artifacts in individual instruments, such as the overestimation of m/z 44 from organic aerosol. This effect was quantified by the m/z (mass-to-charge) 44 to nitrate ratio measured during ammonium nitrate calibrations, with values ranging from 0.03 to 0.26, showing that it can be significant for some instruments. The fragmentation table correction previously proposed to account for this artifact was applied to the measurements acquired during this study. For some instruments (those with high artifacts), this fragmentation table adjustment led to an “overcorrection” of the f44 (m/z 44/Org) signal. This correction based on measurements made with pure NH4NO3, assumes that the magnitude of the artifact is independent of chemical composition. Using data acquired at different NH4NO3 mixing ratios (from solutions of NH4NO3 and (NH4)2SO4) we observe that the magnitude of the artifact varies as a function of composition. Here we applied an updated correction, dependent on the ambient NO3 mass fraction, which resulted in an improved agreement in organic signal among instruments. This work illustrates the benefits of integrating new calibration procedures and artifact corrections, but also highlights the benefits of these intercomparison exercises to continue to improve our knowledge of how these instruments operate, and assist us in interpreting atmospheric chemistry. © 2019, © 2019 Author(s). Published with license by Taylor & Francis Group, LLC.
- ItemIce-Crystal Nucleation in Water: Thermodynamic Driving Force and Surface Tension. Part I: Theoretical Foundation(Basel : MDPI, 2020) Hellmuth, Olaf; Schmelzer, Jürn W.P.; Feistel, RainerA recently developed thermodynamic theory for the determination of the driving force of crystallization and the crystal–melt surface tension is applied to the ice-water system employing the new Thermodynamic Equation of Seawater TEOS-10. The deviations of approximative formulations of the driving force and the surface tension from the exact reference properties are quantified, showing that the proposed simplifications are applicable for low to moderate undercooling and pressure differences to the respective equilibrium state of water. The TEOS-10-based predictions of the ice crystallization rate revealed pressure-induced deceleration of ice nucleation with an increasing pressure, and acceleration of ice nucleation by pressure decrease. This result is in, at least, qualitative agreement with laboratory experiments and computer simulations. Both the temperature and pressure dependencies of the ice-water surface tension were found to be in line with the le Chatelier–Braun principle, in that the surface tension decreases upon increasing degree of metastability of water (by decreasing temperature and pressure), which favors nucleation to move the system back to a stable state. The reason for this behavior is discussed. Finally, the Kauzmann temperature of the ice-water system was found to amount TK=116K , which is far below the temperature of homogeneous freezing. The Kauzmann pressure was found to amount to pK=−212MPa , suggesting favor of homogeneous freezing on exerting a negative pressure on the liquid. In terms of thermodynamic properties entering the theory, the reason for the negative Kauzmann pressure is the higher mass density of water in comparison to ice at the melting point.
- 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.