Preprints
https://doi.org/10.5194/amt-2020-494
https://doi.org/10.5194/amt-2020-494

  18 Dec 2020

18 Dec 2020

Review status: a revised version of this preprint was accepted for the journal AMT.

Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers

Mingyi Wang1,2,, Xu-Cheng He3,, Henning Finkenzeller4, Siddharth Iyer3, Dexian Chen1,5, Jiali Shen3, Mario Simon6, Victoria Hofbauer1,2, Jasper Kirkby6,7, Joachim Curtius6, Norbert Maier8, Theo Kurtén3,8, Douglas R. Worsnop3,9, Markku Kulmala3,10,11,12, Matti Rissanen3,13, Rainer Volkamer4, Yee Jun Tham3, Neil M. Donahue1,2,5,14, and Mikko Sipilä3 Mingyi Wang et al.
  • 1Center for Atmospheric Particle Studies, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
  • 2Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
  • 3Institute for Atmospheric and Earth System Research (INAR), University of Helsinki, 00014 Helsinki, Finland
  • 4Department of Chemistry & CIRES, University of Colorado Boulder, Boulder, CO 80309, USA
  • 5Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
  • 6Institute for Atmospheric and Environmental Sciences, Goethe University Frankfurt, 60438 Frankfurt am Main, Germany
  • 7CERN, the European Organization for Nuclear Research, CH-1211 Geneve 23, Switzerland
  • 8Department of Chemistry, University of Helsinki, 00014 Helsinki, Finland
  • 9Aerodyne Research, Inc., Billerica, MA, 01821, USA
  • 10Helsinki Institute of Physics, P.O. Box 64 (Gustaf Hallstromin katu 2), FI-00014 University of Helsinki, Finland
  • 11Joint International Research Laboratory of Atmospheric and Earth System Sciences, Nanjing University, Nanjing, China
  • 12Aerosol and Haze Laboratory, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China
  • 13Aerosol Physics Laboratory, Physics Unit, Faculty of Engineering and Natural Sciences, Tampere University, Tampere, Finland
  • 14Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, PA, 15213, USA
  • These authors contributed equally to this work.

Abstract. Iodine species are important in the marine atmosphere for oxidation and new-particle formation. Understanding iodine chemistry and iodine new-particle formation requires high time resolution, high sensitivity, and simultaneous measurements of many iodine species. Here, we describe the application of bromide chemical ionization mass spectrometers (Br-CIMS) to this task. During iodine new-particle formation experiments in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber, we have measured gas-phase iodine species and sulfuric acid using two Br-CIMS, one coupled to a Multi-scheme chemical IONization inlet (Br-MION-CIMS) and the other to a Filter Inlet for Gasses and AEROsols inlet (Br-FIGAERO-CIMS). From offline calibrations and inter-comparisons with other instruments attached to the CLOUD chamber, we have quantified the sensitivities of the Br-MION-CIMS to HOI, I2, and H2SO4 and obtain detection limits of 5.8 × 106, 6.3 × 105, and 2.0 × 105 molec cm−3, respectively, for a 2-min integration time. From binding energy calculations, we estimate the detection limit for HIO3 to be 1.2 × 105 molec cm−3, based on an assumption of maximum sensitivity. Detection limits in the Br-FIGAERO-CIMS are around one order of magnitude higher than those in the Br-MION-CIMS; for example, the detection limits for HOI and HIO3 are 3.3 × 107 and 5.1 × 106 molec cm−3, respectively. Our comparisons of the performance of the MION inlet and the FIGAERO inlet show that bromide chemical ionization mass spectrometers using either atmospheric pressure or reduced pressure interfaces are well-matched to measuring iodine species and sulfuric acid in marine environments.

Mingyi Wang et al.

 
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Status: final response (author comments only)
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Mingyi Wang et al.

Mingyi Wang et al.

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Short summary
Atmospheric iodine species are often short-lived with low abundance, thus have been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and the reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec cm−3.