Imaging of transition charge densities involving carbon core excitations by all X-ray sum-frequency generation
Imaging of transition charge densities involving carbon core excitations by all X-ray sum-frequency generation
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通过所有 X 射线和频生成对涉及碳核激发的跃迁电荷密度进行成像
DOI：
10.1098/rsta.2017.0470
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Mukamel, Shaul
中科院分区：
文献类型：
--
作者：
Cho, Daeheum;Rouxel, Jérémy R.;Kowalewski, Markus;Lee, JinYong;Mukamel, Shaul
计算了由化学不等价碳原子的选择性核心激发引起的随时间变化的分子电荷密度的X射线衍射信号。窄带X射线脉冲选择性地激发氟代乙烷（CH 3-CH 2F）中-CH 3或-CH 2F基团的碳K边。每个激发产生一个独特的核心相干性，这取决于电子跃迁的性质。直接传播的减少单电子密度矩阵，使用实时的时间依赖的密度泛函理论，提供了随时间变化的电荷密度以下与外部场的相互作用。部分填充的价分子轨道之间的相互作用在核心激发诱导特征飞秒电荷迁移，这取决于核心-价相干性，并通过和频产生衍射信号进行监测。这篇文章是主题“测量超快电子和结构动力学与X射线”的一部分。
X-ray diffraction signals from the time-evolving molecular charge density induced by selective core excitation of chemically inequivalent carbon atoms are calculated. A narrowband X-ray pulse selectively excites the carbon K-edge of the –CH3or –CH2F groups in fluoroethane (CH3–CH2F). Each excitation creates a distinct core coherence which depends on the character of the electronic transition. Direct propagation of the reduced single-electron density matrix, using real-time time-dependent density functional theory, provides the time-evolving charge density following interactions with external fields. The interplay between partially filled valence molecular orbitals upon core excitation induces characteristic femtosecond charge migration which depends on the core–valence coherence, and is monitored by the sum-frequency generation diffraction signal.This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.
利用瞬态运动方程耦合团簇理论模拟近边缘 X 射线吸收精细结构。
DOI：
10.1021/acs.jpclett.7b01206
发表时间：
2017
期刊：
The journal of physical chemistry letters
影响因子：
--
作者：
Daniel R. Nascimento;A. DePrince
通讯作者：
A. DePrince
纳米光非局部响应张量的平移和旋转平均
DOI：
10.1088/1361-6455/aa9d66
发表时间：
2018
期刊：
Molecular and Optical Physics
影响因子：
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作者：
Rouxel, Jérémy R;Chernyak, Vladimir Y;Mukamel, Shaul
通讯作者：
Mukamel, Shaul