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Title: Toward a chemical reanalysis in a coupled chemistry-climate model: An evaluation of MOPITT CO assimilation and its impact on tropospheric composition

Here, we examine in detail a 1 year global reanalysis of carbon monoxide (CO) that is based on joint assimilation of conventional meteorological observations and Measurement of Pollution in The Troposphere (MOPITT) multispectral CO retrievals in the Community Earth System Model (CESM). Our focus is to assess the impact to the chemical system when CO distribution is constrained in a coupled full chemistry-climate model like CESM. To do this, we first evaluate the joint reanalysis (MOPITT Reanalysis) against four sets of independent observations and compare its performance against a reanalysis with no MOPITT assimilation (Control Run). We then investigate the CO burden and chemical response with the aid of tagged sectoral CO tracers. We estimate the total tropospheric CO burden in 2002 (from ensemble mean and spread) to be 371 ± 12% Tg for MOPITT Reanalysis and 291 ± 9% Tg for Control Run. Our multispecies analysis of this difference suggests that (a) direct emissions of CO and hydrocarbons are too low in the inventory used in this study and (b) chemical oxidation, transport, and deposition processes are not accurately and consistently represented in the model. Increases in CO led to net reduction of OH and subsequent longer lifetime ofmore » CH 4(Control Run: 8.7 years versus MOPITT Reanalysis: 9.3 years). Yet at the same time, this increase led to 5-10% enhancement of Northern Hemisphere O 3 and overall photochemical activity via HO x recycling. Such nonlinear effects further complicate the attribution to uncertainties in direct emissions alone. This has implications to chemistry-climate modeling and inversion studies of longer-lived species.« less
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [3] ;  [3] ;  [3] ;  [1] ;  [1] ;  [1] ;  [4] ;  [1] ;  [5] ;  [6] ;  [7]
  1. National Center for Atmospheric Research, Boulder, CO (United States). Atmospheric Chemistry Observations and Modeling Lab.
  2. Univ. of Arizona, Tucson, AZ (United States). Dept. of Atmospheric Sciences
  3. National Center for Atmospheric Research, Boulder, CO (United States). Inst. for Mathematics Applied to Geosciences
  4. Max Planck Inst. for Chemistry, Mainz (Germany). Biogeochemistry Dept.
  5. Univ. of Bremen (Germany). Inst. of Environmental Physics (IUP)
  6. Univ. of Toronto, ON (Canada). Dept. of Physics
  7. Univ. of Wollongong, NSW (Australia)
Publication Date:
Grant/Contract Number:
AC02-05CH11231; NNX13AK24G; NNX14AN47G; DP110101948; LE0668470
Type:
Accepted Manuscript
Journal Name:
Journal of Geophysical Research: Atmospheres
Additional Journal Information:
Journal Volume: 121; Journal Issue: 12; Journal ID: ISSN 2169-897X
Publisher:
American Geophysical Union
Research Org:
National Center for Atmospheric Research, Boulder, CO (United States); Univ. of Wollongong, NSW (Australia)
Sponsoring Org:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); National Aeronautic and Space Administration (NASA); National Science Foundation (NSF); Australian Research Council (ARC)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; tropospheric composition; data assimilation; chemistry-climate modeling; satellite observations
OSTI Identifier:
1480703

Gaubert, B., Arellano, A. F., Barré, J., Worden, H. M., Emmons, L. K., Tilmes, S., Buchholz, R. R., Vitt, F., Raeder, K., Collins, N., Anderson, J. L., Wiedinmyer, C., Martinez Alonso, S., Edwards, D. P., Andreae, M. O., Hannigan, J. W., Petri, C., Strong, K., and Jones, N.. Toward a chemical reanalysis in a coupled chemistry-climate model: An evaluation of MOPITT CO assimilation and its impact on tropospheric composition. United States: N. p., Web. doi:10.1002/2016JD024863.
Gaubert, B., Arellano, A. F., Barré, J., Worden, H. M., Emmons, L. K., Tilmes, S., Buchholz, R. R., Vitt, F., Raeder, K., Collins, N., Anderson, J. L., Wiedinmyer, C., Martinez Alonso, S., Edwards, D. P., Andreae, M. O., Hannigan, J. W., Petri, C., Strong, K., & Jones, N.. Toward a chemical reanalysis in a coupled chemistry-climate model: An evaluation of MOPITT CO assimilation and its impact on tropospheric composition. United States. doi:10.1002/2016JD024863.
Gaubert, B., Arellano, A. F., Barré, J., Worden, H. M., Emmons, L. K., Tilmes, S., Buchholz, R. R., Vitt, F., Raeder, K., Collins, N., Anderson, J. L., Wiedinmyer, C., Martinez Alonso, S., Edwards, D. P., Andreae, M. O., Hannigan, J. W., Petri, C., Strong, K., and Jones, N.. 2016. "Toward a chemical reanalysis in a coupled chemistry-climate model: An evaluation of MOPITT CO assimilation and its impact on tropospheric composition". United States. doi:10.1002/2016JD024863. https://www.osti.gov/servlets/purl/1480703.
@article{osti_1480703,
title = {Toward a chemical reanalysis in a coupled chemistry-climate model: An evaluation of MOPITT CO assimilation and its impact on tropospheric composition},
author = {Gaubert, B. and Arellano, A. F. and Barré, J. and Worden, H. M. and Emmons, L. K. and Tilmes, S. and Buchholz, R. R. and Vitt, F. and Raeder, K. and Collins, N. and Anderson, J. L. and Wiedinmyer, C. and Martinez Alonso, S. and Edwards, D. P. and Andreae, M. O. and Hannigan, J. W. and Petri, C. and Strong, K. and Jones, N.},
abstractNote = {Here, we examine in detail a 1 year global reanalysis of carbon monoxide (CO) that is based on joint assimilation of conventional meteorological observations and Measurement of Pollution in The Troposphere (MOPITT) multispectral CO retrievals in the Community Earth System Model (CESM). Our focus is to assess the impact to the chemical system when CO distribution is constrained in a coupled full chemistry-climate model like CESM. To do this, we first evaluate the joint reanalysis (MOPITT Reanalysis) against four sets of independent observations and compare its performance against a reanalysis with no MOPITT assimilation (Control Run). We then investigate the CO burden and chemical response with the aid of tagged sectoral CO tracers. We estimate the total tropospheric CO burden in 2002 (from ensemble mean and spread) to be 371 ± 12% Tg for MOPITT Reanalysis and 291 ± 9% Tg for Control Run. Our multispecies analysis of this difference suggests that (a) direct emissions of CO and hydrocarbons are too low in the inventory used in this study and (b) chemical oxidation, transport, and deposition processes are not accurately and consistently represented in the model. Increases in CO led to net reduction of OH and subsequent longer lifetime of CH4(Control Run: 8.7 years versus MOPITT Reanalysis: 9.3 years). Yet at the same time, this increase led to 5-10% enhancement of Northern Hemisphere O3 and overall photochemical activity via HOx recycling. Such nonlinear effects further complicate the attribution to uncertainties in direct emissions alone. This has implications to chemistry-climate modeling and inversion studies of longer-lived species.},
doi = {10.1002/2016JD024863},
journal = {Journal of Geophysical Research: Atmospheres},
number = 12,
volume = 121,
place = {United States},
year = {2016},
month = {5}
}