Abstract

Abstract. Methane (CH4) is both a greenhouse gas and a precursor of tropospheric ozone, making it an important focus of chemistry–climate interactions. Methane has both anthropogenic and natural emission sources, and reaction with the atmosphere's principal oxidizing agent, the hydroxyl radical (OH), is the dominant tropospheric loss process of methane. The tight coupling between methane and OH abundances drives indirect linkages between methane and other short-lived air pollutants and prompts the use of interactive methane chemistry in global chemistry–climate modeling. In this study, an updated contemporary inventory of natural methane emissions and the soil sink is developed using an optimization procedure that applies published emissions data to the NASA GISS ModelE2-Yale Interactive terrestrial Biosphere (ModelE2-YIBs) global chemistry–climate model. Methane observations from the global surface air-sampling network of the Earth System Research Laboratory (ESRL) of the US National Oceanic and Atmospheric Administration (NOAA) are used to guide refinement of the natural methane inventory. The wetland methane flux is calculated as a best fit; thus, the accuracy of this derived flux assumes accurate simulation of methane chemical loss in the atmosphere and accurate prescription of the other methane fluxes (anthropogenic and natural). The optimization process indicates global annual wetland methane emissions of 140 Tg CH4 yr−1. The updated inventory includes total global annual methane emissions from natural sources of 181 Tg CH4 yr−1 and a global annual methane soil sink of 60 Tg CH4 yr−1. An interactive methane simulation is run using ModelE2-YIBs, applying dynamic methane emissions and the updated natural methane emissions inventory that results from the optimization process. The simulated methane chemical lifetime of 10.4±0.1 years corresponds well to observed lifetimes. The simulated year 2005 global-mean surface methane concentration is 1.1 % higher than the observed value from the NOAA ESRL measurements. Comparison of the simulated atmospheric methane distribution with the NOAA ESRL surface observations at 50 measurement locations finds that the simulated annual methane mixing ratio is within 1 % (i.e., +1 % to −1 %) of the observed value at 76 % of locations. Considering the 50 stations, the mean relative difference between the simulated and observed annual methane mixing ratio is a model overestimate of only 0.5 %. Comparison of simulated annual column-averaged methane concentrations with SCIAMACHY satellite retrievals provides an independent post-optimization evaluation of modeled methane. The comparison finds a slight model underestimate in 95 % of grid cells, suggesting that the applied methane source in the model is slightly underestimated or the model's methane sink strength is slightly too strong outside of the surface layer. Overall, the strong agreement between simulated and observed methane lifetimes and concentrations indicates that the ModelE2-YIBs chemistry–climate model is able to capture the principal processes that control atmospheric methane.

Highlights

  • Atmospheric methane (CH4) is a greenhouse gas that warms the climate by absorbing terrestrial radiation

  • The total global annual methane emissions magnitude in E2005 is 532 Tg CH4 yr−1, taking into account the natural flux inventory, anthropogenic emissions derived from the gas–Air pollution Interactions and Synergies (GAINS) integrated assessment model (Amann et al, 2011), and biomass burning and international shipping emissions from the RCP8.5 scenario (Riahi et al, 2011)

  • The good model– measurement agreement indicates that the interactive chemistry scheme in the ModelE2-YIBs global chemistry–climate model, when forced with the updated natural methane flux inventory, appropriately represents the principal chemical and physical processes that affect atmospheric methane, providing confidence in the model’s ability to appropriately capture the methane response to perturbations in emissions of both methane and other short-lived air pollutants

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Summary

Introduction

Atmospheric methane (CH4) is a greenhouse gas that warms the climate by absorbing terrestrial radiation. Observations of methyl chloroform abundance, in conjunction with estimates of methyl chloroform emissions, provide a means to estimate global OH abundance, methyl chloroform lifetime, and, subsequently, methane lifetime (Prinn et al, 1995) Together, these estimates provide a constraint on the total methane flux into the atmosphere; apportionment of this total into contributions from the individual source sectors is highly uncertain (Kirschke et al, 2013; Saunois et al, 2016). The NASA ModelE2-Yale Interactive terrestrial Biosphere (ModelE2YIBs) global chemistry–climate model (Schmidt et al, 2014; Shindell et al, 2013; Yue and Unger, 2015) is subsequently used to run an interactive methane simulation representative of year 2005 that applies the refined natural methane flux inventory. Because methane is an ozone precursor, a comparison of simulated ozone mixing ratios with a contemporary ozone climatology is presented

Interactive methane in ModelE2-YIBs
Model description
Simulation configuration
Contemporary natural methane emissions and soil sink
20 Global
Simulated methane in ModelE2-YIBs
Comparison with surface measurements
Comparison with satellite retrievals
Methane lifetime
Simulated ozone in ModelE2-YIBs
Findings
Conclusions
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