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DOI	10.5194/acp-19-13355-2019
	Rate enhancement in collisions of sulfuric acid molecules due to long-range intermolecular forces
	Halonen R.; Zapadinsky E.; Kurtén T.; Vehkamäki H.; Reischl B.
发表日期	2019
ISSN	16807316
起始页码	13355
结束页码	13366
卷号	19 期号:21
英文摘要	Collisions of molecules and clusters play a key role in determining the rate of atmospheric new particle formation and growth. Traditionally the statistics of these collisions are taken from kinetic gas theory assuming spherical noninteracting particles, which may significantly underestimate the collision coefficients for most atmospherically relevant molecules. Such systematic errors in predicted new particle formation rates will also affect large-scale climate models. We studied the statistics of collisions of sulfuric acid molecules in a vacuum using atomistic molecular dynamics simulations. We found that the effective collision cross section of the H2SO4 molecule, as described by an optimized potentials for liquid simulation (OPLS). OPLS all-atom force field, is significantly larger than the hard-sphere diameter assigned to the molecule based on the liquid density of sulfuric acid. As a consequence, the actual collision coefficient is enhanced by a factor of 2.2 at 300 K compared with kinetic gas theory. This enhancement factor obtained from atomistic simulation is consistent with the discrepancy observed between experimental formation rates of clusters containing sulfuric acid and calculated formation rates using hard-sphere kinetics. We find reasonable agreement with an enhancement factor calculated from the Langevin model of capture, based on the attractive part of the atomistic intermolecular potential of mean force. © 2019 Author(s).
语种	英语
scopus关键词	aerosol formation; atmospheric gas; climate modeling; computer simulation; force; reaction kinetics; sulfuric acid
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/144065
作者单位	Institute for Atmospheric and Earth System Research/Physics, Faculty of Science, University of Helsinki, P.O. Box 64, Helsinki, 00014, Finland; Institute for Atmospheric and Earth System Research/Chemistry, Faculty of Science, University of Helsinki, P.O. Box 55, Helsinki, 00014, Finland
推荐引用方式 GB/T 7714	Halonen R.,Zapadinsky E.,Kurtén T.,et al. Rate enhancement in collisions of sulfuric acid molecules due to long-range intermolecular forces[J],2019,19(21).
APA	Halonen R.,Zapadinsky E.,Kurtén T.,Vehkamäki H.,&Reischl B..(2019).Rate enhancement in collisions of sulfuric acid molecules due to long-range intermolecular forces.Atmospheric Chemistry and Physics,19(21).
MLA	Halonen R.,et al."Rate enhancement in collisions of sulfuric acid molecules due to long-range intermolecular forces".Atmospheric Chemistry and Physics 19.21(2019).