Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)

Abstract

Tropospheric ozone is a major air pollutant and greenhouse gas. It is also the primary precursor of OH, the main tropospheric oxidant. Global atmospheric chemistry models show large differences in their simulations of tropospheric ozone budgets. Here we implement the widely used GEOS-Chem atmospheric chemistry module as an alternative to CAM-chem within the Community Earth System Model version 2 (CESM2). We compare the resulting GEOS-Chem and CAM-chem simulations of tropospheric ozone and related species within CESM2 to observations from ozonesondes, surface sites, the ATom-1 aircraft campaign over the Pacific and Atlantic, and the KORUS-AQ aircraft campaign over the Seoul Metropolitan Area. We find that GEOS-Chem and CAM-chem within CESM2 have similar tropospheric ozone budgets and concentrations usually within 5 ppb but important differences in the underlying processes including (1) photolysis scheme (no aerosol effects in CAM-chem), (2) aerosol nitrate photolysis, (3) N2O5 cloud uptake, (4) tropospheric halogen chemistry, and (5) ozone deposition to the oceans. Global tropospheric OH concentrations are the same in both models, but there are large regional differences reflecting the above processes. Carbon monoxide is lower in CAM-chem (and lower than observations), at least in part because of higher OH concentrations in the Northern Hemisphere and insufficient production from isoprene oxidation in the Southern Hemisphere. CESM2 does not scavenge water-soluble gases in convective updrafts, leading to some upper-tropospheric biases. Comparison to KORUS-AQ observations shows an overestimate of ozone above 4 km altitude in both models, which at least in GEOS-Chem is due to inadequate scavenging of particulate nitrate in convective updrafts in CESM2, leading to excessive NO production from nitrate photolysis. The KORUS-AQ comparison also suggests insufficient boundary layer mixing in CESM2. This implementation and evaluation of GEOS-Chem in CESM2 contribute to the MUSICA vision of modularizing tropospheric chemistry in Earth system models.