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- 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.
- ItemTropospheric Aqueous-Phase Oxidation of Isoprene-Derived Dihydroxycarbonyl Compounds(Washington, DC : Soc., 2017) Otto, Tobias; Stieger, Bastian; Mettke, Peter; Herrmann, HartmutThe dihydroxycarbonyls 3,4-dihydroxy-2-butanone (DHBO) and 2,3-dihydroxy-2-methylpropanal (DHMP) formed from isoprene oxidation products in the atmospheric gas phase under low-NO conditions can be expected to form aqSOA in the tropospheric aqueous phase because of their solubility. In the present study, DHBO and DHMP were investigated concerning their radical-driven aqueous-phase oxidation reaction kinetics. For DHBO and DHMP the following rate constants at 298 K are reported: k(OH + DHBO) = (1.0 ± 0.1) × 109 L mol-1 s-1, k(NO3 + DHBO) = (2.6 ± 1.6) × 106 L mol-1 s-1, k(SO4-+ DHBO) = (2.3 ± 0.2) × 107 L mol-1 s-1, k(OH + DHMP) = (1.2 ± 0.1) × 109 L mol-1 s-1, k (NO3 + DHMP) = (7.9 ± 0.7) × 106 L mol-1 s-1, k(SO4- + DHMP) = (3.3 ± 0.2) × 107 L mol-1 s-1, together with their respective temperature dependences. The product studies of both DHBO and DHMP revealed hydroxydicarbonyls, short chain carbonyls, and carboxylic acids, such as hydroxyacetone, methylglyoxal, and lactic and pyruvic acid as oxidation products with single yields up to 25%. The achieved carbon balance was 75% for DHBO and 67% for DHMP. An aqueous-phase oxidation scheme for both DHBO and DHMP was developed on the basis of the experimental findings to show their potential to contribute to the aqSOA formation. It can be expected that the main contribution to aqSOA occurs via acid formation while other short-chain oxidation products are expected to back-partition into the gas phase to undergo further oxidation there.