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arXiv · 2009.12579

Theory on polarization-averaged core-level molecular-frame photoelectron angular distributions: II. Extracting the X-ray induced fragmentation dynamics of carbon monoxide dication from forward and backward intensities

Fukiko Ota·Keisuke Hatada·D Sébilleau·Kiyoshi Ueda·Kaoru Yamazaki
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Abstract

Recent developments of high-reputation-rate X-ray free electron lasers (XFELs) such as European XFEL and LSCS-II, combined with coincidence measurements at the COLTRIMS-Reaction Microscope, is now opening a door to realize a long-standing dream to create molecular movies of photo-induced chemical reactions of gas-phase molecules. In this paper, we theoretically propose a new method to experimentally visualize dissociation of diatomic molecules via time-resolved polarization-averaged molecular-frame photoelectron angular distributions (PA-MFPADs) measurements using the COLTRIMs--Reaction Microscope and two-color XFEL pump-probe set-up. The first and second order scattering theories with the Muffin-tin approximation give us simple EXAFS type formula for the forward and backward scattering peaks in the PA-MFPADs structure. This formula acts as an experimentally applicable "bond length ruler" by adjusting only three semi-empirical parameters from the time-resolved measurements. The accuracy and applicability of a new ruler equation are numerically examined against the PA-MFPADs of CO 2+ calculated by Full-potential multiple scattering theory as a function of the C-O bond length reported in the preceding work. The bond lengths retrieved from the PA-MFPADs via the EXAFS formula well reproduce the original C-O bond lengths used in the reference ab-initio PA-MFPADs with accuracy of 0.1 Å. We expect that time-resolved PA-MFPADs will be a new attractive tool to make molecular movies visualizing intramolecular reactions.

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Fukiko Ota, Keisuke Hatada, D Sébilleau, Kiyoshi Ueda, Kaoru Yamazaki. 2020-11-14. Theory on polarization-averaged core-level molecular-frame photoelectron angular distributions: II. Extracting the X-ray induced fragmentation dynamics of carbon monoxide dication from forward and backward intensities. https://doi.org/10.1088/1361-6455%2Fabcfd8

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