气候变化领域集成服务门户(CCPortal): An evaluation of global organic aerosol schemes using airborne observations

CCPortal

DOI	10.5194/acp-20-2637-2020
	An evaluation of global organic aerosol schemes using airborne observations
	Pai S.J.; Heald C.L.; Pierce J.R.; Farina S.C.; Marais E.A.; Jimenez J.L.; Campuzano-Jost P.; Nault B.A.; Middlebrook A.M.; Coe H.; Shilling J.E.; Bahreini R.; Dingle J.H.; Vu K.
发表日期	2020
ISSN	1680-7316
起始页码	2637
结束页码	2665
卷号	20 期号:5
英文摘要	Chemical transport models have historically struggled to accurately simulate the magnitude and variability of observed organic aerosol (OA), with previous studies demonstrating that models significantly underestimate observed concentrations in the troposphere. In this study, we explore two different model OA schemes within the standard GEOS-Chem chemical transport model and evaluate the simulations against a suite of 15 globally distributed airborne campaigns from 2008 to 2017, primarily in the spring and summer seasons. These include the ATom, KORUS-AQ, GoAmazon, FRAPPE, SEAC4RS, SENEX, DC3, CalNex, OP3, EUCAARI, ARCTAS and ARCPAC campaigns and provide broad coverage over a diverse set of atmospheric composition regimes - anthropogenic, biogenic, pyrogenic and remote. The schemes include significant differences in their treatment of the primary and secondary components of OA - a "simple scheme" that models primary OA (POA) as non-volatile and takes a fixed-yield approach to secondary OA (SOA) formation and a "complex scheme" that simulates POA as semi-volatile and uses a more sophisticated volatility basis set approach for non-isoprene SOA, with an explicit aqueous uptake mechanism to model isoprene SOA. Despite these substantial differences, both the simple and complex schemes perform comparably across the aggregate dataset in their ability to capture the observed variability (with an R2 of 0.41 and 0.44, respectively). The simple scheme displays greater skill in minimizing the overall model bias (with a normalized mean bias of 0.04 compared to 0.30 for the complex scheme). Across both schemes, the model skill in reproducing observed OA is superior to previous model evaluations and approaches the fidelity of the sulfate simulation within the GEOS-Chem model. However, there are significant differences in model performance across different chemical source regimes, classified here into seven categories. Higher-resolution nested regional simulations indicate that model resolution is an important factor in capturing variability in highly localized campaigns, while also demonstrating the importance of well-constrained emissions inventories and local meteorology, particularly over Asia. Our analysis suggests that a semi-volatile treatment of POA is superior to a non-volatile treatment. It is also likely that the complex scheme parameterization overestimates biogenic SOA at the global scale. While this study identifies factors within the SOA schemes that likely contribute to OA model bias (such as a strong dependency of the bias in the complex scheme on relative humidity and sulfate concentrations), comparisons with the skill of the sulfate aerosol scheme in GEOS-Chem indicate the importance of other drivers of bias, such as emissions, transport and deposition, that are exogenous to the OA chemical scheme. © 2020 BMJ Publishing Group. All rights reserved.
语种	英语
scopus关键词	aerosol; aerosol composition; airborne survey; atmospheric chemistry; biogenic deposit; concentration (composition); organic matter; relative humidity; sulfate; troposphere
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/247940
作者单位	Department of Civil and Environmental Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, United States; Department of Earth, Atmospheric and Planetary Sciences, Massachusetts Institute of Technology, Cambridge, MA 02139, United States; Department of Atmospheric Science, Colorado State University, Fort Collins, CO 80523, United States; Department of Physics and Astronomy, University of Leicester, Leicester, LE1 7RH, United Kingdom; Department of Chemistry, Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, CO 80309, United States; Noaa Earth System Research Laboratory (ESRL), Chemical Sciences Division, 325 Broadway, Boulder, CO 80305, United States; Centre for Atmospheric Science, School of Earth and Environmental Science, University of Manchester, Manchester, M13 9PL, United Kingdom; Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland, WA, United States; Department of Environmental ...
推荐引用方式 GB/T 7714	Pai S.J.,Heald C.L.,Pierce J.R.,et al. An evaluation of global organic aerosol schemes using airborne observations[J],2020,20(5).
APA	Pai S.J..,Heald C.L..,Pierce J.R..,Farina S.C..,Marais E.A..,...&Vu K..(2020).An evaluation of global organic aerosol schemes using airborne observations.ATMOSPHERIC CHEMISTRY AND PHYSICS,20(5).
MLA	Pai S.J.,et al."An evaluation of global organic aerosol schemes using airborne observations".ATMOSPHERIC CHEMISTRY AND PHYSICS 20.5(2020).