Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction

Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

doi:10.1063/1.4984241

Title: Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction

Journal Article · Fri May 26 00:00:00 EDT 2017 · Structural Dynamics

DOI:https://doi.org/10.1063/1.4984241· OSTI ID:1429610

Kowalewski, Markus ^[1]; Bennett, Kochise ^[2]; Mukamel, Shaul ^[2]

Univ. of California, Irvine, CA (United States). Chemistry Dept.
Univ. of California, Irvine, CA (United States). Chemistry Dept. and Dept. of Physics and Astronomy

We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified, representing (in decreasing strength) elastic scattering, contributions of the electronic coherences created by nonadiabatic couplings in the avoided crossing regime, and inelastic scattering. The former probes the charge density and delivers direct information on the evolving molecular geometry. The latter two contributions are weaker and carry spatial information through the transition charge densities (off-diagonal elements of the charge-density operator). Furthermore, simulations are presented for the nonadiabatic harpooning process in the excited state of sodium fluoride.

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Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; Alexander von Humboldt Foundation (Germany)

Grant/Contract Number:: FG02-04ER15571

OSTI ID:: 1429610

Alternate ID(s):: OSTI ID: 1361914

Journal Information:: Structural Dynamics, Vol. 4, Issue 5; ISSN 2329-7778

Publisher:: American Crystallographic Association/AIPCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 43 works

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Title: Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction

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