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Phosgene in the Upper Troposphere and Lower Stratosphere: A Marker for Product Gas Injection Due to Chlorine-Containing Very Short Lived Substances

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posted on 2019-05-22, 15:43 authored by JJ Harrison, MP Chipperfield, R Hossaini, CD Boone, S Dhomse, W Feng, PF Bernath
Phosgene in the atmosphere is produced via the degradation of carbon tetrachloride, methyl chloroform, and a number of chlorine-containing very short lived substances (VSLS). These VSLS are not regulated by the Montreal Protocol even though they contribute to stratospheric ozone depletion. While observations of VSLS can quantify direct stratospheric source gas injection, observations of phosgene in the upper troposphere/lower stratosphere can be used as a marker of product gas injection of chlorine-containing VSLS. In this work we report upper troposphere/lower stratosphere measurements of phosgene made by the ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) instrument and compare with results from the TOMCAT/SLIMCAT three-dimensional chemical transport model to constrain phosgene trends over the 2004–2016 period. The 13-year ACE-FTS time series provides the first observational evidence for an increase in chlorine product gas injection. In 2016, VSLS accounted for 27% of modeled stratospheric phosgene, up from 20% in the mid-2000s.

Funding

This study was funded as part of the UK Research and Innovation Natural Environment Research Council's support of the National Centre for Earth Observation, contract number PR140015. The ACE satellite mission is funded primarily by the Canadian Space Agency (CSA). M. P. Chipperfield is a Royal Society Wolfson Research Merit Award holder. R. Hossaini is supported by a NERC Independent Research Fellowship (NE/N014375/1). We thank the ECMWF for providing the ERA‐Interim reanalyses used by the TOMCAT model. The modeling work used the Archer and Leeds ARC HPC facilities and was supported by the NERC SISLAC project (NE/R001782/1).

History

Citation

Geophysical Research Letters, 2019, 46(2), pp. 1032-1039

Author affiliation

/Organisation/COLLEGE OF SCIENCE AND ENGINEERING/Department of Physics and Astronomy

Version

  • VoR (Version of Record)

Published in

Geophysical Research Letters

Publisher

American Geophysical Union (AGU), Wiley

issn

0094-8276

eissn

1944-8007

Acceptance date

2018-11-03

Copyright date

2018

Available date

2019-05-22

Publisher version

https://agupubs.onlinelibrary.wiley.com/doi/full/10.1029/2018GL079784

Notes

ACE‐FTS data were obtained from https://databace.scisat.ca/level2/ace_v3.5_v3.6/. The TOMCAT model data are available at http://see.leeds.ac.uk/~lecmc/ftp/COCL2.

Language

en

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