Ultrafast x-ray pump x-ray probe transient absorption spectroscopy: A computational study and proposed experiment probing core-valence electronic correlations in solvated complexes

Liekhus-Schmaltz, Chelsea E.; Ho, Phay J.; Weakly, Robert B.; Aquila, Andrew; Schoenlein, Robert W.; Khalil, Munira; Govind, Niranjan

doi:10.1063/5.0047381

Title: Ultrafast x-ray pump x-ray probe transient absorption spectroscopy: A computational study and proposed experiment probing core-valence electronic correlations in solvated complexes

Journal Article · Wed Jun 02 00:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0047381· OSTI ID:1785528

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Univ. of Washington, Seattle, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Institute
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Femtosecond x-ray pump–x-ray probe experiments are currently possible at free electron lasers such as the linac coherent light source, which opens new opportunities for studying solvated transition metal complexes. In order to make the most effective use of these kinds of experiments, it is necessary to determine which chemical properties an x-ray probe pulse will measure. We have combined electron cascade calculations and excited-state time-dependent density functional theory calculations to predict the initial state prepared by an x-ray pump and the subsequent x-ray probe spectra at the Fe K-edge in the solvated model transition metal complex, K4FeII(CN)6. We find several key spectral features that report on the ligand-field splitting and the 3p and 3d electron interactions. We then show how these features could be measured in an experiment.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; KC-030105172685; SC0019277; AC02-76SF00515; AC02-06CH11357; DGE-1762114; AC05-76RL1830

OSTI ID:: 1785528

Alternate ID(s):: OSTI ID: 1785569; OSTI ID: 1813451; OSTI ID: 1820155

Report Number(s):: PNNL-SA-160027; TRN: US2212318

Journal Information:: Journal of Chemical Physics, Vol. 154, Issue 21; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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