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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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Discussion papers
https://doi.org/10.5194/amt-2018-425
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-2018-425
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 12 Dec 2018

Research article | 12 Dec 2018

Review status
This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Measurement Techniques (AMT).

Using collision-induced dissociation to constrain sensitivity of ammonia chemical ionization mass spectrometry (NH4+-CIMS) to oxygenated volatile organic compounds

Alexander Zaytsev1, Martin Breitenlechner1, Abigail R. Koss2, Christopher Y. Lim2, James C. Rowe2, Jesse H. Kroll2, and Frank N. Keutsch1,3,4 Alexander Zaytsev et al.
  • 1John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
  • 2Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA
  • 3Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA
  • 4Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138, USA

Abstract. Chemical ionization mass spectrometers (CIMS) routinely detect hundreds of oxidized organic compounds in the atmosphere. A major limitation of these instruments is the uncertainty in their sensitivity to many of the detected ions. We describe the development of a new high-resolution time-of-flight chemical ionization mass spectrometer that operates in one of two ionization modes: using either ammonium ion ligand switching reactions as NH4+-CIMS or proton transfer reactions as PTR-MS. Switching between the modes can be done within two minutes. The NH4+-CIMS mode of the new instrument has sensitivities of up to 67000dcpsppbv−1 (duty cycle corrected ion counts per second/parts per billion by volume) and detection limits between 1 and 60pptv at 2σ for a 1s integration time for numerous oxygenated volatile organic compounds. We present a mass spectrometric voltage scanning procedure based on collision-induced dissociation that allows us to determine the stability of ammonium-organic ions detected by the NH4+-CIMS. Using this procedure, we can effectively constrain the sensitivity of the ammonia chemical ionization mass-spectrometer to a wide range of detected oxidized volatile organic compounds for which no calibration standards exist. We demonstrate the application of this procedure by quantifying the composition of secondary organic aerosols in a series of laboratory experiments.

Alexander Zaytsev et al.
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Alexander Zaytsev et al.
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Short summary
We present the development of a chemical ionization mass spectrometer which can be operated with either hydronium (H3O+) or ammonium (NH4+) as the reagent ion. We describe a mass spectrometric voltage scanning procedure based on collision-induced dissociation that allows us to determine the stability of detected ammonium-organic ions and hence constrain the sensitivity of the instrument to a wide range of organic compounds that cannot be calibrated directly.
We present the development of a chemical ionization mass spectrometer which can be operated with...
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