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Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Phosgene in the upper troposphere and lower stratosphere
T2 - a marker for product gas injection due to chlorine-containing very short-lived substances
AU - Harrison, Jeremy J.
AU - Chipperfield, Martyn P.
AU - Hossaini, Ryan
AU - Boone, Christopher D.
AU - Dhomse, Sandip
AU - Feng, Wuhu
AU - Bernath, Peter F.
PY - 2019/1/28
Y1 - 2019/1/28
N2 - 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 (SGI), observations of phosgene in the upper troposphere/lower stratosphere (UTLS) can be used as a marker of product gas injection (PGI) of chlorine-containing VSLS. In this work we report UTLS 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 thirteen-year ACE-FTS time series provides the first observational evidence for an increase in chlorine PGI. In 2016, VSLS accounted for 27% of modelled stratospheric phosgene, up from 20% in the mid-2000s.
AB - 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 (SGI), observations of phosgene in the upper troposphere/lower stratosphere (UTLS) can be used as a marker of product gas injection (PGI) of chlorine-containing VSLS. In this work we report UTLS 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 thirteen-year ACE-FTS time series provides the first observational evidence for an increase in chlorine PGI. In 2016, VSLS accounted for 27% of modelled stratospheric phosgene, up from 20% in the mid-2000s.
KW - chlorine
KW - stratosphere
KW - upper troposphere
KW - phosgene
KW - very short-lived substances
KW - carbon tetrachloride
U2 - 10.1029/2018GL079784
DO - 10.1029/2018GL079784
M3 - Journal article
VL - 46
SP - 1032
EP - 1039
JO - Geophysical Research Letters
JF - Geophysical Research Letters
SN - 0094-8276
IS - 2
ER -