Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction

doi:10.1126/science.abb2235

GSTDTAP > 气候变化

DOI	10.1126/science.abb2235
	Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction
	Jie Yang; Xiaolei Zhu; J. Pedro F. Nunes; Jimmy K. Yu; Robert M. Parrish; Thomas J. A. Wolf; Martin Centurion; Markus Gühr; Renkai Li; Yusong Liu; Bryan Moore; Mario Niebuhr; Suji Park; Xiaozhe Shen; Stephen Weathersby; Thomas Weinacht; Todd J. Martinez; Xijie Wang
	2020-05-22
发表期刊	Science
出版年	2020
英文摘要	Because of the complex, ultrafast interplay between nuclear and electronic degrees of freedom, probing both nuclear and electronic dynamics in excited electronic states within a single time-resolved experiment is a great challenge. Yang et al. used ultrafast electron diffraction in combination with ab initio nonadiabatic molecular dynamics and diffraction simulations to study the relaxation dynamics of isolated pyridine molecules after photoexcitation to the S1 state (see the Perspective by Domcke and Sobolewski). They showed that electronic state evolution and molecular structural changes can be recorded simultaneously and independently by tracing a transient signal in small-angle inelastic scattering and large-angle elastic diffraction, respectively. Science , this issue p. [885][1]; see also p. [820][2] Simultaneous observation of nuclear and electronic motion is crucial for a complete understanding of molecular dynamics in excited electronic states. It is challenging for a single experiment to independently follow both electronic and nuclear dynamics at the same time. Here we show that ultrafast electron diffraction can be used to simultaneously record both electronic and nuclear dynamics in isolated pyridine molecules, naturally disentangling the two components. Electronic state changes (S1→S internal conversion) were reflected by a strong transient signal in small-angle inelastic scattering, and nuclear structural changes (ring puckering) were monitored by large-angle elastic diffraction. Supported by ab initio nonadiabatic molecular dynamics and diffraction simulations, our experiment provides a clear view of the interplay between electronic and nuclear dynamics of the photoexcited pyridine molecule. [1]: /lookup/doi/10.1126/science.abb2235 [2]: /lookup/doi/10.1126/science.abb9937
领域	气候变化 ; 资源环境
URL	查看原文
引用统计	被引频次：91[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://119.78.100.173/C666/handle/2XK7JSWQ/270499
专题	气候变化资源环境科学
推荐引用方式 GB/T 7714	Jie Yang,Xiaolei Zhu,J. Pedro F. Nunes,et al. Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction[J]. Science,2020.
APA	Jie Yang.,Xiaolei Zhu.,J. Pedro F. Nunes.,Jimmy K. Yu.,Robert M. Parrish.,...&Xijie Wang.(2020).Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction.Science.
MLA	Jie Yang,et al."Simultaneous observation of nuclear and electronic dynamics by ultrafast electron diffraction".Science (2020).