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Titel |
Optimal estimation of the surface fluxes of methyl chloride using a 3-D global chemical transport model |
VerfasserIn |
X. Xiao, R. G. Prinn, P. J. Fraser, P. G. Simmonds, R. F. Weiss, S. O'Doherty, B. R. Miller, P. K. Salameh, C. M. Harth, P. B. Krummel, L. W. Porter, J. Mühle, B. R. Greally, D. Cunnold, R. Wang, S. A. Montzka, J. W. Elkins, G. S. Dutton, T. M. Thompson, J. H. Butler, B. D. Hall, S. Reimann, M. K. Vollmer, F. Stordal, C. Lunder, M. Maione, J. Arduini, Y. Yokouchi |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 10, no. 12 ; Nr. 10, no. 12 (2010-06-22), S.5515-5533 |
Datensatznummer |
250008567
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Publikation (Nr.) |
copernicus.org/acp-10-5515-2010.pdf |
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Zusammenfassung |
Methyl chloride (CH3Cl) is a chlorine-containing trace gas in the
atmosphere contributing significantly to stratospheric ozone depletion.
Large uncertainties in estimates of its source and sink magnitudes and
temporal and spatial variations currently exist. GEIA inventories and other
bottom-up emission estimates are used to construct a priori maps of the
surface fluxes of CH3Cl. The Model of Atmospheric Transport and
Chemistry (MATCH), driven by NCEP interannually varying meteorological data,
is then used to simulate CH3Cl mole fractions and quantify the time
series of sensitivities of the mole fractions at each measurement site to
the surface fluxes of various regional and global sources and sinks. We then
implement the Kalman filter (with the unit pulse response method) to
estimate the surface fluxes on regional/global scales with monthly
resolution from January 2000 to December 2004. High frequency observations
from the AGAGE, SOGE, NIES, and NOAA/ESRL HATS in situ networks and low
frequency observations from the NOAA/ESRL HATS flask network are used to
constrain the source and sink magnitudes. The inversion results indicate
global total emissions around 4100 ± 470 Gg yr−1 with very large
emissions of 2200 ± 390 Gg yr−1 from tropical plants, which turn
out to be the largest single source in the CH3Cl budget. Relative to
their a priori annual estimates, the inversion increases global annual
fungal and tropical emissions, and reduces the global oceanic source. The
inversion implies greater seasonal and interannual oscillations of the
natural sources and sink of CH3Cl compared to the a priori. The
inversion also reflects the strong effects of the 2002/2003 globally
widespread heat waves and droughts on global emissions from tropical plants,
biomass burning and salt marshes, and on the soil sink. |
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