Volume 228, 2021

Determination of excited state molecular structures from time-resolved gas-phase X-ray scattering

Abstract

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.

Graphical abstract: Determination of excited state molecular structures from time-resolved gas-phase X-ray scattering

Associated articles

Article information

Article type
Paper
Submitted
12 Oct 2020
Accepted
12 Nov 2020
First published
18 Nov 2020

Faraday Discuss., 2021,228, 104-122

Determination of excited state molecular structures from time-resolved gas-phase X-ray scattering

H. Yong, A. Moreno Carrascosa, L. Ma, B. Stankus, M. P. Minitti, A. Kirrander and P. M. Weber, Faraday Discuss., 2021, 228, 104 DOI: 10.1039/D0FD00118J

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