Journal
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES
Volume 123, Issue 18, Pages 10774-10795Publisher
AMER GEOPHYSICAL UNION
DOI: 10.1029/2018JD028388
Keywords
hydroxyl radical; methane lifetime; oxidizing capacity; tropospheric chemistry; climate change
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Funding
- NASA Modeling and Analysis Program
- Aura Science Team
- Atmospheric Composition and Modeling and Analysis Program
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The oxidizing capacity of the troposphere is controlled primarily by the abundance of hydroxyl radical (OH). The global mean concentration of tropospheric OH, [OH](TROP) (the burden of OH in the global troposphere appropriate for calculating the lifetime of methane) inferred from measurements of methyl chloroform has remained relatively constant during the past several decades despite rising levels of methane that should have led to a decline. Here we examine other factors that may have affected [OH](TROP) such as the changing values of stratospheric ozone, rising tropospheric H2O, varying burden of NOx (=NO+NO2), rising temperatures, and widening of the climatological tropics due to expansion of the Hadley cell. Our analysis suggests the positive trends in [OH](TROP) due to H2O, NOx, and overhead O-3, and tropical expansion are large enough ( [OH](TROP)=+0.950.18%/decade) to counter almost all of the expected decrease in [OH](TROP) due to rising methane ( [OH](TROP)=-1.010.05%/decade) over the period 1980 to 2015, while variations in temperature contribute almost no trend ( [OH](TROP)=-0.020.02%/decade) in [OH](TROP). The approximated impact of Hadley cell expansion on [OH](TROP) is also a small but not insignificant factor partially responsible for the steadiness of tropospheric oxidizing capacity over the past several decades, which free-running models likely do not capture.
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