Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport

ATMOSPHERIC CHEMISTRY AND PHYSICS(2023)

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摘要
Atmospheric methane (CH4) concentrations are rising, which are expected to lead to a corresponding increase in the global seasonal cycle amplitude (SCA) - the difference between its seasonal maximum and minimum values. The reaction between CH4 and its main sink, OH, is dependent on the amount of CH4 and OH in the atmosphere. The concentration of OH varies seasonally, and due to the increasing burden of CH4 in the atmosphere, it is expected that the SCA of CH4 will increase due to the increased removal of CH4 through a reaction with OH in the atmosphere. Spatially varying changes in the SCA could indicate long-term persistent variations in the seasonal sources and sinks, but such SCA changes have not been investigated. Here we use surface flask measurements and a 3D chemical transport model (TOMCAT) to diagnose changes in the SCA of atmospheric CH4 between 1995-2020 and attribute the changes regionally to contributions from different sectors. We find that the observed SCA decreased by 4 ppb (7.6 %) in the northern high latitudes (NHLs; 60-90 degrees N), while the SCA increased globally by 2.5 ppb (6.5 %) during this time period. TOMCAT reproduces the change in the SCA at observation sites across the globe. Therefore, we use it to attribute regions which are contributing to the changes in the NHL SCA, which shows an unexpected change in the SCA that differs from the rest of the world. We find that well-mixed background CH4, likely from emissions originating in, and transported from, more southerly latitudes has the largest impact on the decreasing SCA in the NHLs (56.5% of total contribution to NHLs). In addition to the background CH4, recent emissions from Canada, the Middle East, and Europe contribute 16.9 %, 12.1 %, and 8.4 %, respectively, to the total change in the SCA in the NHLs. The remaining contributions are due to changes in emissions and transport from other regions. The three largest regional contributions are driven by increases in summer emissions from the Boreal Plains in Canada, decreases in winter emissions across Europe, and a combination of increases in summer emissions and decreases in winter emissions over the Arabian Peninsula and Caspian Sea in the Middle East. These results highlight that changes in the observed seasonal cycle can be an indicator of changing emission regimes in local and non-local regions, particularly in the NHL, where the change is counterintuitive.
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northern high latitudes,seasonal cycle amplitude,methane,emissions,lower-latitude
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