气候变化领域集成服务门户(CCPortal): Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations

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DOI	10.5194/acp-19-10073-2019
	Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations
	Evoy E.; Maclean A.M.; Rovelli G.; Li Y.; Tsimpidi A.P.; Karydis V.A.; Kamal S.; Lelieveld J.; Shiraiwa M.; Reid J.P.; Bertram A.K.
发表日期	2019
ISSN	16807316
起始页码	10073
结束页码	10085
卷号	19 期号:15
英文摘要	Information on the rate of diffusion of organic molecules within secondary organic aerosol (SOA) is needed to accurately predict the effects of SOA on climate and air quality. Diffusion can be important for predicting the growth, evaporation, and reaction rates of SOA under certain atmospheric conditions. Often, researchers have predicted diffusion rates of organic molecules within SOA using measurements of viscosity and the Stokes-Einstein relation (D ∝ 1/η, where D is the diffusion coefficient and η is viscosity). However, the accuracy of this relation for predicting diffusion in SOA remains uncertain. Using rectangular area fluorescence recovery after photobleaching (rFRAP), we determined diffusion coefficients of fluorescent organic molecules over 8 orders in magnitude in proxies of SOA including citric acid, sorbitol, and a sucrose-citric acid mixture. These results were combined with literature data to evaluate the Stokes-Einstein relation for predicting the diffusion of organic molecules in SOA. Although almost all the data agree with the Stokes-Einstein relation within a factor of 10, a fractional Stokes-Einstein relation (D ∝ 1/ηξ) with ξ = 0:93 is a better model for predicting the diffusion of organic molecules in the SOA proxies studied. In addition, based on the output from a chemical transport model, the Stokes-Einstein relation can overpredict mixing times of organic molecules within SOA by as much as 1 order of magnitude at an altitude of ∼ 3 km compared to the fractional Stokes-Einstein relation with ξ = 0.93. These results also have implications for other areas such as in food sciences and the preservation of biomolecules. © Author(s) 2019.
语种	英语
scopus关键词	accuracy assessment; aerosol; air quality; atmospheric chemistry; atmospheric transport; diffusion; numerical method; organic matter; prediction
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/144226
作者单位	Department of Chemistry, University of British Columbia, 2036 Main Mall, Vancouver, BC V6T 1Z1, Canada; School of Chemistry, University of Bristol, Bristol, BS8 1TS, United Kingdom; Department of Chemistry, University of California, Irvine, CA 92697-2025, United States; Atmospheric Chemistry Department, Max Planck Institute for Chemistry, Mainz, 55128, Germany; National Observatory of Athens, Institute for Environmental Research and Sustainable Development, Palea Penteli, 15236, Greece; Forschungszentrum Jülich, Institute of Energy and Climate Research, IEK-8, Jülich, 52425, Germany; Energy, Environment and Water Research Center, Cyprus Institute, Nicosia, 1645, Cyprus; Chemical Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94611, United States
推荐引用方式 GB/T 7714	Evoy E.,Maclean A.M.,Rovelli G.,et al. Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations[J],2019,19(15).
APA	Evoy E..,Maclean A.M..,Rovelli G..,Li Y..,Tsimpidi A.P..,...&Bertram A.K..(2019).Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations.Atmospheric Chemistry and Physics,19(15).
MLA	Evoy E.,et al."Predictions of diffusion rates of large organic molecules in secondary organic aerosols using the Stokes-Einstein and fractional Stokes-Einstein relations".Atmospheric Chemistry and Physics 19.15(2019).