Double core hole valence-to-core x-ray emission spectroscopy: A theoretical exploration using time-dependent density functional theory

Zhang, Yu; Bergmann, Uwe; Schoenlein, Robert; Khalil, Munira; Govind, Niranjan

doi:10.1063/1.5111141

Title: Double core hole valence-to-core x-ray emission spectroscopy: A theoretical exploration using time-dependent density functional theory

Journal Article · Fri Oct 11 00:00:00 EDT 2019 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5111141· OSTI ID:1591640

^[1];

^[2]; Schoenlein, Robert ^[3];

^[4];

^[5]

SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.
SLAC National Accelerator Lab., Menlo Park, CA (United States). LCLS and Stanford PULSE Inst.
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Univ. of Washington, Seattle, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

With the help of newly developed X-ray free-electron laser (XFEL) sources, creating double core holes (DCHs) simultaneously at the same or different atomic sites in a molecule has now become possible. DCH X-ray emission is a new form of X-ray nonlinear spectroscopy that can be studied with a XFEL. Here in this paper, we computationally explore the metal K-edge valence-to-core (VtC) X-ray emission spectroscopy (XES) of metal/metal and metal/ligand DCH states in a series of transition metal complexes with time-dependent density functional theory. The simulated DCH VtC-XES signals are compared with conventional single core hole (SCH) XES signals. The energy shifts and intensity changes of the DCH emission lines with respect to the corresponding SCH-XES features are fingerprints of the coupling between the second core hole and the occupied orbitals around the DCHs that contain important chemical bonding information of the complex. The difference between delocalized/localized core hole models on DCH VtC-XES is also briefly discussed. We theoretically demonstrate that DCH XES provides subtle information on the local electronic structure around metal centers in transition metal complexes beyond conventional linear XES. In conclusion, our predicted changes from calculations between SCH-XES and DCH-XES features should be detectable with modern XFEL sources.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: KC030105172685; SC0019277; AC05-76RL1830; AC02-76SF00515; AC02-05CH11231; AC05-76RL01830

OSTI ID:: 1591640

Alternate ID(s):: OSTI ID: 1570073; OSTI ID: 1608543

Report Number(s):: PNNL-SA-143614; TRN: US2102049

Journal Information:: Journal of Chemical Physics, Vol. 151, Issue 14; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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