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    The 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, Olivier
    This 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.
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    Variations of the aerosol chemical composition during Asian dust storm at Dushanbe, Tajikistan
    (Les Ulis : EDP Sciences, 2019) Fomba, Khanneh Wadinga; Müller, Konrad; Hofer, Julian; Makhmudov, Abduvosit N.; Althausen, Dietrich; Nazarov, Bahron I.; Abdullaev, Sabur F.; Herrmann, Hartmut
    Aerosol chemical composition was characterized during the Central Asian Dust Experiment (CADEX) at Dushanbe (Tajikistan). Aerosol samples were collected during a period of 2 months from March to May 2015 using a high volume DIGITEL DHA-80 sampler on quartz fiber filters. The filters were analyzed for their ionic, trace metals as well as organic and elemental carbon (OC/EC) content. The aerosol mass showed strong variation with mass concentration ranging from 18 μg/m3 to 110 μg/m3. The mineral dust concentrations varied between 0.9 μg/m3 and 88 μg/m3. Days of high aerosol mass loadings were dominated by mineral dust, which made up to about 80% of the aerosol mass while organic matter and inorganic ions made up about 70% of the aerosol mass during days of low aerosol mass loadings. The mineral dust composition showed different trace metal signatures in comparison to Saharan dust with higher Ca content and Ca/Fe ratios twice as high as that observed in Saharan dust. Strong influence of anthropogenic activities was observed in the trace metal concentrations with Zn and Pb concentrations ranging from 7 to 197 ng/m3 and 2 to 20 ng/m3, respectively. Mineral dust and anthropogenic activities relating to traffic, combustion as well as metallurgical industrial emissions are identified as the sources of the aerosol during this period. © 2019 The Authors, published by EDP Sciences.
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    Dust impacts on radiative effects of black carbon aerosol in Central Asia
    (Les Ulis : EDP Sciences, 2019) Tegen, Ina; Heinold, Bernd
    The radiative effect of mineral dust and black carbon aerosol are investigated with aerosolclimate model simulations with fixed sea surface temperatures as boundary condition. The semi-direct effects of the absorbing aerosol are assessed as the residual between the total direct radiative effect and the instantaneous direct radiative effect of the aerosol species. For Central Asia the presence of mineral dust aerosol below a black carbon aerosol layer enhances the positive radiative effect of the black carbon aerosol. © 2019 The Authors, published by EDP Sciences.
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    Aerosol layer heights above Tajikistan during the CADEX campaign
    (Les Ulis : EDP Sciences, 2019) Hofer, Julian; Althausen, Dietrich; Abdullaev, Sabur F.; Nazarov, Bakhron I.; Makhmudov, Abduvosit N.; Baars, Holger; Engelmann, Ronny; Ansmann, Albert
    Mineral dust influences climate and weather by direct and indirect effects. Surrounded by dust sources, Central Asian countries are affected by atmospheric mineral dust on a regular basis. Climate change effects like glacier retreat and desertification are prevalent in Central Asia as well. Therefore, the role of dust in the climate system in Central Asia needs to be clarified and quantified. During the Central Asian Dust EXperiment (CADEX) first lidar observations in Tajikistan were conducted. Long-term vertically resolved aerosol measurements were performed with the multiwavelength polarization Raman lidar PollyXT from March 2015 to August 2016 in Dushanbe, Tajikistan. In this contribution, a climatology of the aerosol layer heights is presented, which was retrieved from the 18-month lidar measurements. Automatic detection based on backscatter coefficient thresholds were used to retrieve the aerosol layer heights and yield similar layer heights as manual layer height determination. The significant aerosol layer height has a maximum in summer and a minimum in winter. The highest layers occurred in spring, but in summer uppermost layer heights above 6 km AGL are frequent, too. © 2019 The Authors, published by EDP Sciences.
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    Vertical profiles of dust and other aerosol types above a coastal site
    (Les Ulis : EDP Sciences, 2019) Althausen, Dietrich; Mewes, Silke; Heese, Birgit; Hofer, Julian; Schechner, Yoav; Aides, Amit; Holodovsky, Vadim
    Monthly mean vertical profiles of aerosol type occurrences are determined from multiwavelength Raman and polarization lidar measurements above Haifa, Israel, in 2017. This contribution presents the applied methods and threshold values. The results are discussed for one example, May 2017. This month shows more often large, non-spherical particles in lofted layers than within the planetary boundary layer. Small particles are observed at higher altitudes only when they are observed in lower altitudes, too. © 2019 The Authors, published by EDP Sciences.
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    Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol
    (Washington, DC : ACS Publ., 2019) Bianchi, Federico; Kurtén, Theo; Riva, Matthieu; Mohr, Claudia; Rissanen, Matti P.; Roldin, Pontus; Berndt, Torsten; Crounse, John D.; Wennberg, Paul O.; Mentel, Thomas F.; Wildt, Jürgen; Junninen, Heikki; Jokinen, Tuija; Kulmala, Markku; Worsnop, Douglas R.; Thornton, Joel A.; Donahue, Neil; Kjaergaard, Henrik G.; Ehn, Mikael
    Highly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earth's radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research. © 2019 American Chemical Society.
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    Tropospheric aqueous-phase chemistry: kinetics, mechanisms, and its coupling to a changing gas phase
    (Washington, DC : ACS Publ., 2015) Herrmann, Hartmut; Schaefer, Thomas; Tilgner, Andreas; Styler, Sarah A.; Weller, Christian; Teich, Monique; Otto, Tobias
    [no abstract available]
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    The ocean's vital skin: Toward an integrated understanding of the sea surface microlayer
    (Lausanne : Frontiers Media, 2017) Engel, Anja; Bange, Hermann W.; Cunliffe, Michael; Burrows, Susannah M.; Friedrichs, Gernot; Galgani, Luisa; Herrmann, Hartmut; Hertkorn, Norbert; Johnson, Martin; Liss, Peter S.; Quinn, Patricia K.; Schartau, Markus; Soloviev, Alexander; Stolle, Christian; Upstill-Goddard, Robert C.; van Pinxteren, Manuela; Zäncker, Birthe
    Despite the huge extent of the ocean's surface, until now relatively little attention has been paid to the sea surface microlayer (SML) as the ultimate interface where heat, momentum and mass exchange between the ocean and the atmosphere takes place. Via the SML, large-scale environmental changes in the ocean such as warming, acidification, deoxygenation, and eutrophication potentially influence cloud formation, precipitation, and the global radiation balance. Due to the deep connectivity between biological, chemical, and physical processes, studies of the SML may reveal multiple sensitivities to global and regional changes. Understanding the processes at the ocean's surface, in particular involving the SML as an important and determinant interface, could therefore provide an essential contribution to the reduction of uncertainties regarding ocean-climate feedbacks. This review identifies gaps in our current knowledge of the SML and highlights a need to develop a holistic and mechanistic understanding of the diverse biological, chemical, and physical processes occurring at the ocean-atmosphere interface. We advocate the development of strong interdisciplinary expertise and collaboration in order to bridge between ocean and atmospheric sciences. Although this will pose significant methodological challenges, such an initiative would represent a new role model for interdisciplinary research in Earth System sciences.
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    Variability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations
    (Amsterdam [u.a.] : Elsevier Science, 2018) Sun, J.; Birmili, W.; Hermann, M.; Tuch, T.; Weinhold, K.; Spindler, G.; Schladitz, A.; Bastian, S.; Löschau, G.; Cyrys, J.; Gu, J.; Flentje, H.; Briel, B.; Asbac, C.; Kaminski, H.; Ries, L.; Sohme, R.; Gerwig, H.; Wirtz, K.; Meinhardt, F.; Schwerin, A.; Bath, O.; Ma, N.; Wiedensohler, A.
    This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors
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    Do new sea spray aerosol source functions improve the results of a regional aerosol model?
    (Amsterdam [u.a.] : Elsevier Science, 2018) Barthel, Stefan; Tegen, Ina; Wolke, Ralf
    Sea spray aerosol particle is a dominating part of the global aerosol mass load of natural origin. Thus, it strongly influences the atmospheric radiation balance and cloud properties especially over the oceans. Uncertainties of the estimated climate impacts by this aerosol type are partly caused by the uncertainties in the particle size dependent emission fluxes of sea spray aerosol particle. We present simulations with a regional aerosol transport model system in two domains, for three months and compared the model results to measurements at four stations using various sea spray aerosol particle source source functions. Despite these limitations we found the results using different source functions are within the range of most model uncertainties. Especially the model's ability to produce realistic wind speeds is crucial. Furthermore, the model results are more affected by a function correcting the emission flux for the effect of the sea surface temperature than by the use of different source functions. © 2018 The Authors