Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations

Global and regional methane budgets are markedly uncertain. Conventionally, estimates of methane sources are derived by bridging emissions inventories with atmospheric observations employing chemical transport models. The accuracy of this approach requires correctly simulating advection and chem...

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Main Authors: K. M. Saad, D. Wunch, N. M. Deutscher, D. W. T. Griffith, F. Hase, M. De Mazière, J. Notholt, D. F. Pollard, C. M. Roehl, M. Schneider, R. Sussmann, T. Warneke, P. O. Wennberg
Format: Article
Language:English
Published: Copernicus Publications 2016-11-01
Series:Atmospheric Chemistry and Physics
Online Access:https://www.atmos-chem-phys.net/16/14003/2016/acp-16-14003-2016.pdf
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spelling doaj-adb2697110de4745b1f06280ac8577e12020-11-25T00:09:43ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242016-11-0116140031402410.5194/acp-16-14003-2016Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observationsK. M. Saad0D. Wunch1D. Wunch2N. M. Deutscher3N. M. Deutscher4D. W. T. Griffith5F. Hase6M. De Mazière7J. Notholt8D. F. Pollard9C. M. Roehl10M. Schneider11R. Sussmann12T. Warneke13P. O. Wennberg14Environmental Science and Engineering, California Institute of Technology, Pasadena, California, USAEnvironmental Science and Engineering, California Institute of Technology, Pasadena, California, USADepartment of Physics, University of Toronto, Toronto, Ontario, CanadaCenter for Atmospheric Chemistry, School of Chemistry, University of Wollongong, Wollongong, NSW, AustraliaInstitute of Environmental Physics, University of Bremen, Bremen, GermanyCenter for Atmospheric Chemistry, School of Chemistry, University of Wollongong, Wollongong, NSW, AustraliaInstitute for Meteorology and Climate Research, Karlsruhe Institute of Technology, IMK-ASF, Karlsruhe, GermanyRoyal Belgian Institute for Space Aeronomy, Brussels, BelgiumInstitute of Environmental Physics, University of Bremen, Bremen, GermanyNational Institute of Water and Atmospheric Research, Omakau, New ZealandEnvironmental Science and Engineering, California Institute of Technology, Pasadena, California, USAInstitute for Meteorology and Climate Research, Karlsruhe Institute of Technology, IMK-ASF, Karlsruhe, GermanyInstitute for Meteorology and Climate Research, Karlsruhe Institute of Technology, IMK-IFU, Garmisch-Partenkirchen, GermanyInstitute of Environmental Physics, University of Bremen, Bremen, GermanyEnvironmental Science and Engineering, California Institute of Technology, Pasadena, California, USAGlobal and regional methane budgets are markedly uncertain. Conventionally, estimates of methane sources are derived by bridging emissions inventories with atmospheric observations employing chemical transport models. The accuracy of this approach requires correctly simulating advection and chemical loss such that modeled methane concentrations scale with surface fluxes. When total column measurements are assimilated into this framework, modeled stratospheric methane introduces additional potential for error. To evaluate the impact of such errors, we compare Total Carbon Column Observing Network (TCCON) and GEOS-Chem total and tropospheric column-averaged dry-air mole fractions of methane. We find that the model's stratospheric contribution to the total column is insensitive to perturbations to the seasonality or distribution of <i>tropospheric</i> emissions or loss. In the Northern Hemisphere, we identify disagreement between the measured and modeled stratospheric contribution, which increases as the tropopause altitude decreases, and a temporal phase lag in the model's tropospheric seasonality driven by transport errors. Within the context of GEOS-Chem, we find that the errors in tropospheric advection partially compensate for the stratospheric methane errors, masking inconsistencies between the modeled and measured tropospheric methane. These seasonally varying errors alias into source attributions resulting from model inversions. In particular, we suggest that the tropospheric phase lag error leads to large misdiagnoses of wetland emissions in the high latitudes of the Northern Hemisphere.https://www.atmos-chem-phys.net/16/14003/2016/acp-16-14003-2016.pdf
collection DOAJ
language English
format Article
sources DOAJ
author K. M. Saad
D. Wunch
D. Wunch
N. M. Deutscher
N. M. Deutscher
D. W. T. Griffith
F. Hase
M. De Mazière
J. Notholt
D. F. Pollard
C. M. Roehl
M. Schneider
R. Sussmann
T. Warneke
P. O. Wennberg
spellingShingle K. M. Saad
D. Wunch
D. Wunch
N. M. Deutscher
N. M. Deutscher
D. W. T. Griffith
F. Hase
M. De Mazière
J. Notholt
D. F. Pollard
C. M. Roehl
M. Schneider
R. Sussmann
T. Warneke
P. O. Wennberg
Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
Atmospheric Chemistry and Physics
author_facet K. M. Saad
D. Wunch
D. Wunch
N. M. Deutscher
N. M. Deutscher
D. W. T. Griffith
F. Hase
M. De Mazière
J. Notholt
D. F. Pollard
C. M. Roehl
M. Schneider
R. Sussmann
T. Warneke
P. O. Wennberg
author_sort K. M. Saad
title Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
title_short Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
title_full Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
title_fullStr Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
title_full_unstemmed Seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
title_sort seasonal variability of stratospheric methane: implications for constraining tropospheric methane budgets using total column observations
publisher Copernicus Publications
series Atmospheric Chemistry and Physics
issn 1680-7316
1680-7324
publishDate 2016-11-01
description Global and regional methane budgets are markedly uncertain. Conventionally, estimates of methane sources are derived by bridging emissions inventories with atmospheric observations employing chemical transport models. The accuracy of this approach requires correctly simulating advection and chemical loss such that modeled methane concentrations scale with surface fluxes. When total column measurements are assimilated into this framework, modeled stratospheric methane introduces additional potential for error. To evaluate the impact of such errors, we compare Total Carbon Column Observing Network (TCCON) and GEOS-Chem total and tropospheric column-averaged dry-air mole fractions of methane. We find that the model's stratospheric contribution to the total column is insensitive to perturbations to the seasonality or distribution of <i>tropospheric</i> emissions or loss. In the Northern Hemisphere, we identify disagreement between the measured and modeled stratospheric contribution, which increases as the tropopause altitude decreases, and a temporal phase lag in the model's tropospheric seasonality driven by transport errors. Within the context of GEOS-Chem, we find that the errors in tropospheric advection partially compensate for the stratospheric methane errors, masking inconsistencies between the modeled and measured tropospheric methane. These seasonally varying errors alias into source attributions resulting from model inversions. In particular, we suggest that the tropospheric phase lag error leads to large misdiagnoses of wetland emissions in the high latitudes of the Northern Hemisphere.
url https://www.atmos-chem-phys.net/16/14003/2016/acp-16-14003-2016.pdf
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