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    Stable 15N isotopes in fine and coarse urban particulate matter
    (Philadelphia, Pa : Taylor & Francis, 2021) Wiedenhaus, Hanna; Ehrnsperger, Laura; Klemm, Otto; Strauss, Harald
    Particulate nitrogen has far-reaching negative effects on human health and the environment, and effective strategies for reducing it require understanding its sources and formation processes. To learn about these factors, we recorded size-resolved nitrogen isotope ratios (δ15N) of total particulate N at an urban site in northwest Germany during a four-week measuring campaign. We observed a steady decrease in δ15N when going from fine to coarse particles, with values between +18 ‰ and −2 ‰. This difference based on particle size is caused by different isotope fractionation processes during particle formation: The fine particles contain ammonium nitrate, which is formed in an equilibrium process, leading to an enrichment of 15N. Moreover, fine particles are more reactive due to their larger surface areas and relatively long residence times in the atmosphere, which leads to an additional enrichment of 15N; a key step of this process likely occurs when the ammonium particles interact with ammonia from agricultural sources. In contrast to fine particles, coarse particles are formed by direct absorption of HNO3 on preexisting particles; the HNO3 stems from traffic emissions of NOx and subsequent oxidation in the atmospheric gas phase. Because only a small amount of isotope fractionation is associated with non-equilibrium processes during phase transitions, there is less 15N enrichment in the coarse particles. Overall, nitrogen isotopes clearly reflect the different formation processes of fine and coarse aerosol particles. © 2021 The Author(s). Published with license by Taylor & Francis Group, LLC.
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    Mobility particle size spectrometers: Calibration procedures and measurement uncertainties
    (Philadelphia, Pa : Taylor & Francis, 2017) Wiedensohler, A.; Wiesner, A.; Weinhold, K.; Birmili, W.; Hermann, M.; Merkel, M.; Müller, T.; Pfeifer, S.; Schmidt, A.; Tuch, T.; Velarde, F.; Quincey, P.; Seeger, S.; Nowak, A.
    Mobility particle size spectrometers (MPSS) belong to the essential instruments in aerosol science that determine the particle number size distribution (PNSD) in the submicrometer size range. Following calibration procedures and target uncertainties against standards and reference instruments are suggested for a complete MPSS quality assurance program: (a) calibration of the CPC counting efficiency curve (within 5% for the plateau counting efficiency; within 1 nm for the 50% detection efficiency diameter), (b) sizing calibration of the MPSS, using a certified polystyrene latex (PSL) particle size standard at 203 nm (within 3%), (c) intercomparison of the PNSD of the MPSS (within 10% and 20% of the dN/dlogDP concentration for the particle size range 20–200 and 200–800 nm, respectively), and (d) intercomparison of the integral PNC of the MPSS (within 10%). Furthermore, following measurement uncertainties have been investigated: (a) PSL particle size standards in the range from 100 to 500 nm match within 1% after sizing calibration at 203 nm. (b) Bipolar diffusion chargers based on the radioactive nuclides Kr85, Am241, and Ni63 and a new ionizer based on corona discharge follow the recommended bipolar charge distribution, while soft X-ray-based charges may alter faster than expected. (c) The use of a positive high voltage supply show a 10% better performance than a negative one. (d) The intercomparison of the integral PNC of an MPSS against the total number concentration is still within the target uncertainty at an ambient pressure of approximately 500 hPa. Copyright © 2018 Published with license by American Association for Aerosol Research.
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    An Overview on the Role of Relative Humidity in Airborne Transmission of SARS-CoV-2 in Indoor Environments
    (Taoyuan City : Taiwan Association for Aerosol Research (TAAR), 2020) Ahlawat, Ajit; Wiedensohler, Alfred; Mishra, Sumit Kumar
    COVID-19 disease is caused by severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), which originated in Wuhan, China and spread with an astonishing rate across the world. The transmission routes of SARS-CoV-2 are still debated, but recent evidence strongly suggests that COVID-19 could be transmitted via air in poorly ventilated places. Some studies also suggest the higher surface stability of SARS-CoV-2 as compared to SARS-CoV-1. It is also possible that small viral particles may enter into indoor environments from the various emission sources aided by environmental factors such as relative humidity, wind speed, temperature, thus representing a type of an aerosol transmission. Here, we explore the role of relative humidity in airborne transmission of SARS-CoV-2 virus in indoor environments based on recent studies around the world. Humidity affects both the evaporation kinematics and particle growth. In dry indoor places i.e., less humidity (< 40% RH), the chances of airborne transmission of SARS-CoV-2 are higher than that of humid places (i.e., > 90% RH). Based on earlier studies, a relative humidity of 40–60% was found to be optimal for human health in indoor places. Thus, it is extremely important to set a minimum relative humidity standard for indoor environments such as hospitals, offices and public transports for minimization of airborne spread of SARS-CoV-2. © The Author(s).
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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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    Separation and quantification of imidazoles in atmospheric particles using LC-Orbitrap-MS
    (Weinheim : Wiley-VCH, 2020) Teich, Monique; Schmidtpott, Mechthild; van Pinxteren, Dominik; Chen, Jianmin; Herrmann, Hartmut
    A method using ultra-high performance liquid chromatography coupled to a high resolution Orbitrap mass spectrometer was developed to identify and quantify imidazoles in aqueous extracts of aerosol particles. The aqueous particle extract was used without further enrichment or sample clean-up. Five columns were tested for efficient separation of ten imidazoles and the Acquity HSS T3 column was chosen for further optimization. Low limits of detection (<25 nM) and good intraday and interday repeatability (<1.6 and <6%, respectively) were achieved. Investigation of matrix effects showed that external calibration is applicable when the loading of organic carbon in the sample is below 10 µg m-3 . The developed method was applied to ten real samples, and six out of the ten test imidazoles were successfully quantified, while six further imidazoles were qualitatively identified, among them 4-imidazolecarboxaldehyde and 4-methyl-5-imidazolecarboxaldehyde. Advantages of the method are the minimal sample preparation, the short run time for each sample, and the low detection limits. These allow for a fast and reliable quantification of imidazoles even in a large number of aqueous particle extract samples.
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    Determination of highly polar compounds in atmospheric aerosol particles at ultra-trace levels using ion chromatography Orbitrap mass spectrometry
    (Weinheim : Wiley-VCH, 2021) Kwiezinski, Carlo; Weller, Christian; van Pinxteren, Dominik; Brüggemann, Martin; Mertes, Stephan; Stratmann, Frank; Herrmann, Hartmut
    A method using ion chromatography coupled to high-resolution Orbitrap mass spectrometry was developed to quantify highly-polar organic compounds in aqueous filter extracts of atmospheric particles. In total, 43 compounds, including short-chain carboxylic acids, terpene-derived acids, organosulfates, and inorganic anions were separated within 33 min by a KOH gradient. Ionization by electrospray was maximized by adding 100 µL min−1 isopropanol as post-column solvent and optimizing the ion source settings. Detection limits (S/N ≥ 3) were in the range of 0.075–25 μg L−1 and better than previously reported for 22 compounds. Recoveries of extraction typically range from 85 to 117%. The developed method was applied to three ambient samples, including two arctic flight samples, and one sample from Melpitz, a continental backround research site. A total of 32 different compounds were identified for all samples. From the arctic flight samples, organic tracers could be quantified for the first time with concentrations ranging from 0.1 to 17.8 ng m−3. Due to the minimal sample preparation, the beneficial figures of merit, and the broad range of accessible compounds, including very polar ones, the new method offers advantages over existing ones and enables a detailed analysis of organic marker compounds in atmospheric aerosol particles.