Determination of excited state molecular structures from time-resolved gas-phase X-ray scattering
Determination of excited state molecular structures from time-resolved gas-phase X-ray scattering
复制标题
利用时间分辨气相 X 射线散射测定激发态分子结构
DOI：
10.1039/d0fd00118j
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发表时间：
2021
影响因子：
3.4
通讯作者：
Weber, Peter M.
中科院分区：
文献类型：
--
作者：
Yong, Haiwang;Moreno Carrascosa, Andrés;Ma, Lingyu;Stankus, Brian;Minitti, Michael P.;Kirrander, Adam;Weber, Peter M.
我们提出了一个全面的调查，最近推出的方法，以确定瞬态结构的分子在激发电子态的亚昂斯特罗姆分辨率从时间分辨的气相散射信号。该方法，这是检查使用时间分辨的X射线散射数据测量的分子N-甲基吗啉（NMM）在直线加速器相干光源（LCLS），比较实验测得的散射图案对模拟图案对应于一个大池的分子结构，以确定完整的结构参数。此外，我们研究了振动态分布的影响，并发现在目前的实验检测限的影响可以忽略不计，尽管分子有一个相对较高的内部振动能。使用三种不同的计算方法产生的三个结构池确定的激发态结构是在良好的协议，表明该程序在很大程度上是独立的计算化学方法，只要池是足够膨胀的附近寻求的结构和密集的足够产生良好的匹配的实验模式。
We present a comprehensive investigation of a recently introduced method to determine transient structures of molecules in excited electronic states with sub-ångstrom resolution from time-resolved gas-phase scattering signals. The method, which is examined using time-resolved X-ray scattering data measured on the molecule N-methylmorpholine (NMM) at the Linac Coherent Light Source (LCLS), compares the experimentally measured scattering patterns against the simulated patterns corresponding to a large pool of molecular structures to determine the full set of structural parameters. In addition, we examine the influence of vibrational state distributions and find the effect negligible within the current experimental detection limits, despite that the molecules have a comparatively high internal vibrational energy. The excited state structures determined using three structure pools generated using three different computational methods are in good agreement, demonstrating that the procedure is largely independent of the computational chemistry method employed as long as the pool is sufficiently expansive in the vicinity of the sought structure and dense enough to yield good matches to the experimental patterns.