Large difference in aerosol radiative effects from BVOC-SOA treatment in three ESMs

Atmospheric Chemistry and Physics(2020)

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摘要
Abstract. Biogenic volatile organic compounds (BVOCs) emitted from vegetation are oxidized 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 past 10 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 results show that the impact on the direct radiative effect (DRE) are linked to the changes in the SOA production in the models, where more SOA leads to a stronger DRE and vice versa. The magnitude by which the DRE changes (maximally 0.15 W m−2 globally averaged) in response to the SOA changes however varies between the models, with EC-Earth displaying the largest changes. The results for the cloud radiative effects (CRE) 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 has 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 parameterization have 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 introduces uncertainty into ESM estimates of aerosol forcing from land-use change and BVOC feedback strengths.
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