Large difference in aerosol radiative effects from BVOC-SOA treatment in three Earth system models

Abstract

Biogenic volatile organic compounds (BVOCs) emitted from vegetation are oxidised in the atmosphere and can form aerosol particles either by contributing to new particle formation or by condensing onto existing aerosol particles. As the understanding of the importance of BVOCs for aerosol formation has increased over the years, these processes have made their way into Earth system models (ESMs). In this study, sensitivity experiments are run with three different ESMs (the Norwegian Earth System Model (NorESM), EC-Earth and ECHAM) to investigate how the direct and indirect aerosol radiative effects are affected by changes in the formation of secondary organic aerosol (SOA) from BVOCs. In the first two sensitivity model experiments, the yields of SOA precursors from oxidation of BVOCs are changed by ±50 %. For the third sensitivity test, the formed oxidation products do not participate in the formation of new particles but are only allowed to condense onto existing aerosols. In the last two sensitivity experiments, the emissions of BVOC compounds (isoprene and monoterpenes) are turned off, one at a time. The goal of the study is to investigate whether it is of importance to treat SOA formation processes correctly in the models rather than to evaluate the correctness of the current treatment in the models. The results show that the impact on the direct radiative effect (DRE) is linked to the changes in the SOA production in the models, where more SOA leads to a stronger DRE and vice versa. However, the magnitude by which the DRE changes (maximally 0.15 W m−2 globally averaged) in response to the SOA changes varies between the models, with EC-Earth displaying the largest changes. The results for the cloud radiative effects (CREs) are more complicated than for the DRE. The changes in CRE differ more among the ESMs, and for some sensitivity experiments they even have different signs. The most sensitive models are NorESM and EC-Earth, which have CRE changes of up to 0.82 W m−2. The varying responses in the different models are connected to where in the aerosol size distributions the changes in mass and number due to SOA formation occur, in combination with the aerosol number concentration levels in the models. We also find that interactive gas-phase chemistry as well as the new particle formation parameterisation has important implications for the DRE and CRE in some of the sensitivity experiments. The results from this study indicate that BVOC-SOA treatment in ESMs can have a substantial impact on the modelled climate but that the sensitivity varies greatly between the models. Since BVOC emissions have changed historically and will continue to change in the future, the spread in model results found in this study implies uncertainty into ESM estimates of aerosol forcing from land-use change and BVOC feedback strengths.