Sebastian V. Pios, Jiaji Zhang, Maxim F. Gelin, Hong-Guang Duan, Lipeng Chen
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引用次数: 0
摘要
X 射线自由电子激光器的发展使得超快 X 射线衍射(XRD)实验成为可能,它能够解析分子中的电子和振动跃迁以及结构变化,或捕捉分子电影。虽然时间分辨 XRD 引起了越来越多的关注,但从信号中提取信息是一项挑战,需要理论支持。在这项工作中,我们结合了 X 射线散射理论和轨迹表面跳跃方法,通过研究电子激发态和基态之间电子密度变化的时间演化,解析了光激发分子电子结构的动态变化。以吡嗪分子为例,我们表明可以识别反应路径的关键特征,从而捕捉光激发分子与电子跃迁相关的结构变化。
Tracking the Electron Density Changes in Excited States: A Computational Study of Pyrazine
The development of X-ray free-electron lasers has enabled ultrafast X-ray diffraction (XRD) experiments, which are capable of resolving electronic and vibrational transitions and structural changes in molecules or capturing molecular movies. While time-resolved XRD has attracted more attention, the extraction of information from signals is challenging and requires theoretical support. In this work, we combined X-ray scattering theory and a trajectory surface hopping approach to resolve dynamical changes in the electronic structure of photoexcited molecules by studying the time evolution of electron density changes between electronic excited states and ground state. Using the pyrazine molecule as an example, we show that key features of reaction pathways can be identified, enabling the capture of structural changes associated with electronic transitions for a photoexcited molecule.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.