Near-Edge X-ray Absorption Fine Structure Spectroscopy of Heteroatomic Core-Hole States as a Probe for Nearly Indistinguishable Chemical Environments

Nascimento, Daniel R.; Zhang, Yu; Bergmann, Uwe; Govind, Niranjan

doi:10.1021/acs.jpclett.9b03500

Title: Near-Edge X-ray Absorption Fine Structure Spectroscopy of Heteroatomic Core-Hole States as a Probe for Nearly Indistinguishable Chemical Environments

Journal Article · 05 January 2020 · Journal of Physical Chemistry Letters

DOI: https://doi.org/10.1021/acs.jpclett.9b03500 · OSTI ID:1605285

^[1]; Zhang, Yu ^[2];

^[2];

^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab.
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)

We demonstrate how the near-edge X-ray absorption fine structure (NEXAFS) spectroscopy of single and double core-hole states created by the ionization of a heteroatom can be used to probe subtle changes in intramolecular chemical environments that are nearly indistinguishable by conventional NEXAFS spectroscopy. Using prototypical organic molecules (2/3-pentanone and pentanal), we show how new spectral features emerge in the C K-edge NEXAFS spectra, when creating single and double core-holes at the oxygen heteroatom site. The effect on the lowest unoccupied molecular orbitals is analyzed by studying the double-core-hole-induced ultrafast valence electron dynamics of the three molecules. The predicted changes from our simulations should be observable with state-of-the-art experiments at X-ray free-electron lasers.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1605285

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 2 Vol. 11; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Energy
Molecules
Oxygen
X-ray absorption near edge spectroscopy
X-rays

Title: Near-Edge X-ray Absorption Fine Structure Spectroscopy of Heteroatomic Core-Hole States as a Probe for Nearly Indistinguishable Chemical Environments

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