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DOI	10.1073/pnas.2105046118
	Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals
	Cavaletto S.M.; Keefer D.; Rouxel J.R.; Aleotti F.; Segatta F.; Garavelli M.; Mukamel S.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:22
英文摘要	The outcomes and timescales of molecular nonadiabatic dynamics are decisively impacted by the quantum coherences generated at localized molecular regions. In time-resolved X-ray diffraction imaging, these coherences create distinct signatures via inelastic photon scattering, but they are buried under much stronger background elastic features. Here, we exploit the rich dynamical information encoded in the inelastic patterns, which we reveal by frequency-dispersed covariance ultrafast powder X-ray diffraction of stochastic X-ray free-electron laser pulses. This is demonstrated for the photoisomerization of azobenzene involving the passage through a conical intersection, where the nuclear wave packet branches and explores different quantum pathways. Snapshots of the coherence dynamics are obtained at high frequency shifts, not accessible with conventional diffraction measurements. These provide access to the timing and to the confined spatial distribution of the valence electrons directly involved in the conical intersection passage. This study can be extended to full threedimensional imaging of conical intersections with ultrafast X-ray and electron diffraction. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Free-electron lasers; Molecular coherences; Nonadiabatic dynamics; X-ray diffraction imaging
语种	英语
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/238537
作者单位	Department of Chemistry, University of California, Irvine, CA 92697, United States; Department of Physics & Astronomy, University of California, Irvine, CA 92697, United States; University Lyon, UJM-Saint- Etienne, CNRS, Graduate School Optics Institute, Laboratoire Hubert Curien UMR 5516, Saint-Etienne, 42023, France; Dipartimento di Chimica Industriale, Universita Degli Studi di Bologna, Bologna, 40136, Italy
推荐引用方式 GB/T 7714	Cavaletto S.M.,Keefer D.,Rouxel J.R.,et al. Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals[J],2021,118(22).
APA	Cavaletto S.M..,Keefer D..,Rouxel J.R..,Aleotti F..,Segatta F..,...&Mukamel S..(2021).Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals.Proceedings of the National Academy of Sciences of the United States of America,118(22).
MLA	Cavaletto S.M.,et al."Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals".Proceedings of the National Academy of Sciences of the United States of America 118.22(2021).