气候变化领域集成服务门户(CCPortal): Future changes in isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) under the Shared Socioeconomic Pathways: The importance of physicochemical dependency

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DOI	10.5194/acp-21-3395-2021
	Future changes in isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) under the Shared Socioeconomic Pathways: The importance of physicochemical dependency
	Jo D.S.; Hodzic A.; Emmons L.K.; Tilmes S.; Schwantes R.H.; Mills M.J.; Campuzano-Jost P.; Hu W.; Zaveri R.A.; Easter R.C.; Singh B.; Lu Z.; Schulz C.; Schneider J.; Shilling J.E.; Wisthaler A.; Jimenez J.L.
发表日期	2021
ISSN	1680-7316
起始页码	3395
结束页码	3425
卷号	21 期号:5
英文摘要	Secondary organic aerosol (SOA) is a dominant contributor of fine particulate matter in the atmosphere, but the complexity of SOA formation chemistry hinders the accurate representation of SOA in models. Volatility-based SOA parameterizations have been adopted in many recent chemistry modeling studies and have shown a reasonable performance compared to observations. However, assumptions made in these empirical parameterizations can lead to substantial errors when applied to future climatic conditions as they do not include the mechanistic understanding of processes but are rather fitted to laboratory studies of SOA formation. This is particularly the case for SOA derived from isoprene epoxydiols (IEPOX SOA), for which we have a higher level of understanding of the fundamental processes than is currently parameterized in most models. We predict future SOA concentrations using an explicit mechanism and compare the predictions with the empirical parameterization based on the volatility basis set (VBS) approach. We then use the Community Earth System Model 2 (CESM2.1.0) with detailed isoprene chemistry and reactive uptake processes for the middle and end of the 21st century under four Shared Socioeconomic Pathways (SSPs): SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5. With the explicit chemical mechanism, we find that IEPOX SOA is predicted to increase on average under all future SSP scenarios but with some variability in the results depending on regions and the scenario chosen. Isoprene emissions are the main driver of IEPOX SOA changes in the future climate, but the IEPOX SOA yield from isoprene emissions also changes by up to 50 % depending on the SSP scenario, in particular due to different sulfur emissions. We conduct sensitivity simulations with and without CO2 inhibition of isoprene emissions that is highly uncer tain, which results in factor of 2 differences in the predicted IEPOX SOA global burden, especially for the high-CO2 scenarios (SSP3-7.0 and SSP5-8.5). Aerosol pH also plays a critical role in the IEPOX SOA formation rate, requiring accurate calculation of aerosol pH in chemistry models. On the other hand, isoprene SOA calculated with the VBS scheme predicts a nearly constant SOA yield from isoprene emissions across all SSP scenarios; as a result, it mostly follows isoprene emissions regardless of region and scenario. This is because the VBS scheme does not consider heterogeneous chemistry; in other words, there is no dependency on aerosol properties. The discrepancy between the explicit mechanism and VBS parameterization in this study is likely to occur for other SOA components as well, which may also have dependencies that cannot be captured by VBS parameterizations. This study highlights the need for more explicit chemistry or for parameterizations that capture the dependence on key physicochemical drivers when predicting SOA concentrations for climate studies. © 2021 Author(s).
语种	英语
scopus关键词	aerosol; isoprene; numerical model; parameterization; particulate matter; physicochemical property; sulfur emission
来源期刊	ATMOSPHERIC CHEMISTRY AND PHYSICS
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/247086
作者单位	Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO, United States; Department of Chemistry, University of Colorado, Boulder, CO, United States; Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO, United States; Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, United States; Department of Atmospheric Sciences, Texas A and M University, College Station, TX, United States; Particle Chemistry Department, Max Planck Institute for Chemistry, Mainz, Germany; Leibniz Institute for Tropospheric Research, Leipzig, Germany; Department of Chemistry, University of Oslo, Oslo, Norway; Institute for Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, Austria; Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, United States; Chemical Sciences Laboratory, National Oceanic and Atmospheric Ad...
推荐引用方式 GB/T 7714	Jo D.S.,Hodzic A.,Emmons L.K.,et al. Future changes in isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) under the Shared Socioeconomic Pathways: The importance of physicochemical dependency[J],2021,21(5).
APA	Jo D.S..,Hodzic A..,Emmons L.K..,Tilmes S..,Schwantes R.H..,...&Jimenez J.L..(2021).Future changes in isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) under the Shared Socioeconomic Pathways: The importance of physicochemical dependency.ATMOSPHERIC CHEMISTRY AND PHYSICS,21(5).
MLA	Jo D.S.,et al."Future changes in isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) under the Shared Socioeconomic Pathways: The importance of physicochemical dependency".ATMOSPHERIC CHEMISTRY AND PHYSICS 21.5(2021).