How Does Tropospheric VOC Chemistry Affect Climate? An Investigation Using the Community Earth System Model Version 2

Abstract. Because of their computational expense, models with comprehensive tropospheric chemistry have typically been run with prescribed sea surface temperatures (SSTs), which greatly limits the model's ability to generate climate responses to atmospheric forcings. In the past few years, however, several fully-coupled models with comprehensive tropospheric chemistry have been developed. For example, the Community Earth System Model version 2 with the Whole Atmosphere Community Climate Model version 6 as its atmospheric component (CESM2-WACCM6) has implemented fully interactive tropospheric chemistry with 231 chemical species as well as a fully coupled ocean. Earlier versions of this model used a "SOAG scheme" that prescribes bulk emission of a single gas-phase precursor to secondary organic aerosols (SOAs). The additional chemistry in CESM2-WACCM6 simulates the chemistry of a comprehensive range of volatile organic compounds (VOCs) responsible for tropospheric aerosol formation. Such a model offers an opportunity to examine the full climate effects of comprehensive tropospheric chemistry. To examine these effects, 141-year preindustrial control simulations were performed using the following two configurations: 1) the standard CESM2-WACCM6 configuration with interactive chemistry over the whole atmosphere (WACtl), and 2) a simplified CESM2-WACCM6 configuration using a SOAG scheme in the troposphere and interactive chemistry in the middle atmosphere (MACtl). The middle atmospheric chemistry is the same in both configurations, and only the tropospheric chemistry differs. Differences between WACtl and MACtl were analyzed for various fields. Regional differences in annual mean surface temperature range between -4 K and 4 K. These surface temperature changes are comparable to those produced over a century in future climate change scenarios, which motivates future research to investigate possible influences of VOC chemistry on anthropogenic climate change. In the zonal average, there is widespread tropospheric cooling in the extratropics. Longwave forcers are shown to be unlikely drivers of this cooling, and possible shortwave forcers are explored. Evidence is presented that the climate response is primarily due to increased organic nitrates in the troposphere, increased sulfate aerosols in the stratosphere and cloud feedbacks. The possible chemical mechanisms responsible for these changes are discussed. As found in earlier studies, enhanced internal mixing with SOAs in WACtl causes reduced black carbon (BC) and reduced primary organic matter (POM), which are not directly influenced by VOC chemistry. These BC and POM reductions might also contribute to cooling in the Northern Hemisphere. The extratropical tropospheric cooling results in dynamical changes, such as equatorward shifts of the midlatitude jets, which in turn drive extratropical changes in clouds and precipitation. In the tropical upper troposphere, cloud-driven increases in shortwave heating appear to weaken and expand the Hadley circulation, which in turn drives changes in tropical and subtropical precipitation.