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DOI	10.1073/pnas.2021714118
	Ultrafast X-ray scattering offers a structural view of excited-state charge transfer
	Yong H.; Xu X.; Ruddock J.M.; Stankus B.; Carrascosa A.M.; Zotev N.; Bellshaw D.; Du W.; Goff N.; Chang Y.; Boutet S.; Carbajo S.; Koglin J.E.; Liang M.; Robinson J.S.; Kirrander A.; Minitti M.P.; Weber P.M.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:19
英文摘要	molecular structure in N,N′-dimethylpiperazine are tracked using femtosecond gas-phase X-ray scattering. The molecules are optically excited to the 3p state at 200 nm. Following rapid relaxation to the 3s state, distinct charge-localized and charge-delocalized species related by charge transfer are observed. The experiment determines the molecular structure of the two species, with the redistribution of electron density accounted for by a scattering correction factor. The initially dominant charge-localized state has a weakened carbon.carbon bond and reorients one methyl group compared with the ground state. Subsequent charge transfer to the charge-delocalized state elongates the carbon.carbon bond further, creating an extended 1.634 Å bond, and also reorients the second methyl group. At the same time, the bond lengths between the nitrogen and the ring-carbon atoms contract from an average of 1.505 to 1.465 Å. The experiment determines the overall charge transfer time constant for approaching the equilibrium between charge-localized and charge-delocalized species to 3.0 ps. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Charge transfer; Excited state; Femtosecond; Ultrafast dynamics; X-ray scattering
语种	英语
scopus关键词	carbon; methyl group; nitrogen; algorithm; anisotropy; Article; chemical bond; chemical structure; conformation; geometry; photoelectron spectroscopy; radiation scattering; structure analysis
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/238571
作者单位	Department of Chemistry, Brown University, Providence, RI 02912, United States; Department of Chemistry and Biochemistry, Western Connecticut State University, Danbury, CT 06810, United States; EaStCHEM, School of Chemistry, University of Edinburgh, Edinburgh, EH9 3FJ, United Kingdom; Center for Science at Extreme Conditions, University of Edinburgh, Edinburgh, EH9 3FJ, United Kingdom; Linac Coherent Light Source, Stanford Linear Accelerator Center National Accelerator Laboratory, Menlo Park, CA 94025, United States
推荐引用方式 GB/T 7714	Yong H.,Xu X.,Ruddock J.M.,et al. Ultrafast X-ray scattering offers a structural view of excited-state charge transfer[J],2021,118(19).
APA	Yong H..,Xu X..,Ruddock J.M..,Stankus B..,Carrascosa A.M..,...&Weber P.M..(2021).Ultrafast X-ray scattering offers a structural view of excited-state charge transfer.Proceedings of the National Academy of Sciences of the United States of America,118(19).
MLA	Yong H.,et al."Ultrafast X-ray scattering offers a structural view of excited-state charge transfer".Proceedings of the National Academy of Sciences of the United States of America 118.19(2021).