Resonant X-ray Sum-Frequency-Generation Spectroscopy of K-Edges in Acetyl Fluoride

Bruner, Adam; Cavaletto, Stefano M.; Govind, Niranjan; Mukamel, Shaul

doi:10.1021/acs.jctc.9b00642

Resonant X-ray Sum-Frequency-Generation Spectroscopy of K-Edges in Acetyl Fluoride

Journal Article · Tue Nov 12 00:00:00 EST 2019 · Journal of Chemical Theory and Computation

DOI:https://doi.org/10.1021/acs.jctc.9b00642· OSTI ID:1922847

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Univ. of California, Irvine, CA (United States); Regents, University of California, Irvine
Univ. of California, Irvine, CA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Resonant X-ray sum-frequency generation is calculated for excitations of the fluorine and the oxygen core K-edge in acetyl fluoride using real-time time-dependent density functional theory. The signal is generated by an extreme-ultraviolet pulse followed by an X-ray pulse with variable delay T. Here, the X-ray pulse is tuned to different element-specific core excitations and used to probe the dynamics of a valence electronic wave packet. A two-dimensional signal is recorded depending on the dispersed X-ray pulse frequency and the frequency conjugated to T, revealing the couplings between core and valence excited states. Molecular orbital decomposition of the signal reveals which regions of the molecule contribute to the X-ray excitation.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: SC0019484

OSTI ID:: 1922847

Alternate ID(s):: OSTI ID: 1580523

Journal Information:: Journal of Chemical Theory and Computation, Journal Name: Journal of Chemical Theory and Computation Journal Issue: 12 Vol. 15; ISSN 1549-9618

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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