Abstract
Abstract. The CH4 growth rate in the atmosphere showed large variations after the Pinatubo eruption in June 1991. A decrease of more than 10 ppb yr−1 in the growth rate over the course of 1992 was reported, and a partial recovery in the following year. Although several reasons have been proposed to explain the evolution of CH4 after the eruption, their contributions to the observed variations are not yet resolved. CH4 is removed from the atmosphere by the reaction with tropospheric OH, which in turn is produced by O3 photolysis under UV radiation. The CH4 removal after the Pinatubo eruption might have been affected by changes in tropospheric UV levels due to the presence of stratospheric SO2 and sulfate aerosols, and due to enhanced ozone depletion on Pinatubo aerosols. The perturbed climate after the eruption also altered both sources and sinks of atmospheric CH4. Furthermore, CH4 concentrations were influenced by other factors of natural variability in that period, such as El Niño–Southern Oscillation (ENSO) and biomass burning events. Emissions of CO, NOX and non-methane volatile organic compounds (NMVOCs) also affected CH4 concentrations indirectly by influencing tropospheric OH levels.Potential drivers of CH4 variability are investigated using the TM5 global chemistry model. The contribution that each driver had to the global CH4 variability during the period 1990 to 1995 is quantified. We find that a decrease of 8–10 ppb yr−1 CH4 is explained by a combination of the above processes. However, the timing of the minimum growth rate is found 6&nash;9 months later than observed. The long-term decrease in CH4 growth rate over the period 1990 to 1995 is well captured and can be attributed to an increase in OH concentrations over this time period. Potential uncertainties in our modelled CH4 growth rate include emissions of CH4 from wetlands, biomass burning emissions of CH4 and other compounds, biogenic NMVOC and the sensitivity of OH to NMVOC emission changes. Two inventories are used for CH4 emissions from wetlands, ORCHIDEE and LPJ, to investigate the role of uncertainties in these emissions. Although the higher climate sensitivity of ORCHIDEE improves the simulated CH4 growth rate change after Pinatubo, none of the two inventories properly captures the observed CH4 variability in this period.
Highlights
Methane (CH4) is the second most important anthropogenic greenhouse gas after carbon dioxide (CO2)
We quantify the combined impact of the drivers of CH4 variability described above in the early 1990s using the TM5 global chemistry and transport model, and we identify the potential gaps in our understanding of the CH4 budget
The 1.6 % inter-annual variability (IAV) we find for the CH4 loss by reaction with OH supports the conclusion of Montzka et al (2011) that OH concentrations are buffered against atmospheric perturbations, having an IAV of about 2 %
Summary
Methane (CH4) is the second most important anthropogenic greenhouse gas after carbon dioxide (CO2). Its evolution in the atmosphere since the beginning of the record of continuous atmospheric CH4 measurements in the 1980s is not fully understood, with large discrepancies between bottom-up and top-down estimates of CH4 sources and sinks (Kirschke et al, 2013). One of the events that affected CH4 concentrations was the eruption of Mt Pinatubo on 15 June 1991, the largest eruption in the last century. The eruption caused perturbations to climate and photochemistry for a few years afterwards. We investigate here the sensitivity of CH4 concentrations to these perturbations and our ability to explain the observed CH4 variations in the atmosphere in the early 1990s
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