气候变化领域集成服务门户(CCPortal): Solvent-mediated electron hopping: long-range charge transfer in IBr-CO2 photodissociation

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DOI	10.1126/science.1184616
	Solvent-mediated electron hopping: long-range charge transfer in IBr-CO2 photodissociation
	Sheps L.; Miller E.M.; Horvath S.; Thompson M.A.; Parson R.; McCoy A.B.; Carl Lineberger W.
发表日期	2010
ISSN	0036-8075
起始页码	220
结束页码	224
卷号	328 期号:5975
英文摘要	Chemical bond breaking involves coupled electronic and nuclear dynamics that can take place on multiple electronic surfaces. Here we report a time-resolved experimental and theoretical investigation of nonadiabatic dynamics during photodissociation of a complex of iodine monobromide anion with carbon dioxide [IBr-(CO2)l on the second excited (A') electronic state. Previous experimental work showed that the dissociation of bare IBr- yields only I- + Br products. However, in IBr -(CO2), time-resolved photoelectron spectroscopy reveals that a subset of the dissociating molecules undergoes an electron transfer from iodine to bromine 350 femtoseconds after the initial excitation. Ab initio calculations and molecular dynamics simulations elucidate the mechanism for this charge hop and highlight the crucial role of the carbon dioxide molecule. The charge transfer between two recoiling atoms, assisted by a single solvent-like molecule, provides a notable limiting case of solvent-driven electron transfer over a distance of 7 angstroms.
英文关键词	bromine; bromine derivative; carbon dioxide; iodine; iodine monobromide; unclassified drug; anion; bromide; carbon dioxide; chemical bonding; electron; experimental study; iodine; molecular analysis; photodegradation; spectroscopy; ab initio calculation; article; dissociation; dynamics; electron; electron transport; excitation; experimental study; molecular dynamics; nonhuman; priority journal; theoretical study; X ray photoelectron spectroscopy
语种	英语
来源期刊	Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/245457
作者单位	JILA, Department of Chemistry and Biochemistry, University of Colorado at Boulder, Boulder, CO 80309, United States; Department of Chemistry, Ohio State University, Columbus, OH 43210, United States; NASA Goddard Space Flight Center, Greenbelt, MD 20771, United States
推荐引用方式 GB/T 7714	Sheps L.,Miller E.M.,Horvath S.,et al. Solvent-mediated electron hopping: long-range charge transfer in IBr-CO2 photodissociation[J],2010,328(5975).
APA	Sheps L..,Miller E.M..,Horvath S..,Thompson M.A..,Parson R..,...&Carl Lineberger W..(2010).Solvent-mediated electron hopping: long-range charge transfer in IBr-CO2 photodissociation.Science,328(5975).
MLA	Sheps L.,et al."Solvent-mediated electron hopping: long-range charge transfer in IBr-CO2 photodissociation".Science 328.5975(2010).