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Title: Chemical Feedback From Decreasing Carbon Monoxide Emissions

Understanding changes in the burden and growth rate of atmospheric methane (CH 4) has been the focus of several recent studies but still lacks scientific consensus. Here we investigate the role of decreasing anthropogenic carbon monoxide (CO) emissions since 2002 on hydroxyl radical (OH) sinks and tropospheric CH 4 loss. We quantify this impact by contrasting two model simulations for 2002–2013: (1) a Measurement of the Pollution in the Troposphere (MOPITT) CO reanalysis and (2) a Control-Run without CO assimilation. These simulations are performed with the Community Atmosphere Model with Chemistry of the Community Earth System Model fully coupled chemistry climate model with prescribed CH 4 surface concentrations. The assimilation of MOPITT observations constrains the global CO burden, which significantly decreased over this period by ~20%. We find that this decrease results to (a) increase in CO chemical production, (b) higher CH 4 oxidation by OH, and (c) ~8% shorter CH 4 lifetime. As a result, we elucidate this coupling by a surrogate mechanism for CO-OH-CH 4 that is quantified from the full chemistry simulations.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1] ;  [3] ; ORCiD logo [3] ; ORCiD logo [1]
  1. National Center for Atmospheric Research, Boulder, CO (United States)
  2. Univ. of Arizona, Tucson, AZ (United States)
  3. SRON Netherlands Institute for Space Research, Utrecht (Netherlands); Utrecht Univ., Utrecht (Netherlands)
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Geophysical Research Letters
Additional Journal Information:
Journal Volume: 44; Journal Issue: 19; Journal ID: ISSN 0094-8276
Publisher:
American Geophysical Union
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; tropospheric composition; data assimilation; global chemistry transport model; chemistry climate modeling; air pollution
OSTI Identifier:
1479337

Gaubert, B., Worden, H. M., Arellano, A. F. J., Emmons, L. K., Tilmes, S., Barré, J., Martinez Alonso, S., Vitt, F., Anderson, J. L., Alkemade, F., Houweling, S., and Edwards, D. P.. Chemical Feedback From Decreasing Carbon Monoxide Emissions. United States: N. p., Web. doi:10.1002/2017GL074987.
Gaubert, B., Worden, H. M., Arellano, A. F. J., Emmons, L. K., Tilmes, S., Barré, J., Martinez Alonso, S., Vitt, F., Anderson, J. L., Alkemade, F., Houweling, S., & Edwards, D. P.. Chemical Feedback From Decreasing Carbon Monoxide Emissions. United States. doi:10.1002/2017GL074987.
Gaubert, B., Worden, H. M., Arellano, A. F. J., Emmons, L. K., Tilmes, S., Barré, J., Martinez Alonso, S., Vitt, F., Anderson, J. L., Alkemade, F., Houweling, S., and Edwards, D. P.. 2017. "Chemical Feedback From Decreasing Carbon Monoxide Emissions". United States. doi:10.1002/2017GL074987. https://www.osti.gov/servlets/purl/1479337.
@article{osti_1479337,
title = {Chemical Feedback From Decreasing Carbon Monoxide Emissions},
author = {Gaubert, B. and Worden, H. M. and Arellano, A. F. J. and Emmons, L. K. and Tilmes, S. and Barré, J. and Martinez Alonso, S. and Vitt, F. and Anderson, J. L. and Alkemade, F. and Houweling, S. and Edwards, D. P.},
abstractNote = {Understanding changes in the burden and growth rate of atmospheric methane (CH4) has been the focus of several recent studies but still lacks scientific consensus. Here we investigate the role of decreasing anthropogenic carbon monoxide (CO) emissions since 2002 on hydroxyl radical (OH) sinks and tropospheric CH4 loss. We quantify this impact by contrasting two model simulations for 2002–2013: (1) a Measurement of the Pollution in the Troposphere (MOPITT) CO reanalysis and (2) a Control-Run without CO assimilation. These simulations are performed with the Community Atmosphere Model with Chemistry of the Community Earth System Model fully coupled chemistry climate model with prescribed CH4 surface concentrations. The assimilation of MOPITT observations constrains the global CO burden, which significantly decreased over this period by ~20%. We find that this decrease results to (a) increase in CO chemical production, (b) higher CH4 oxidation by OH, and (c) ~8% shorter CH4 lifetime. As a result, we elucidate this coupling by a surrogate mechanism for CO-OH-CH4 that is quantified from the full chemistry simulations.},
doi = {10.1002/2017GL074987},
journal = {Geophysical Research Letters},
number = 19,
volume = 44,
place = {United States},
year = {2017},
month = {9}
}