Near-Edge X-ray Absorption Fine Structure Spectroscopy of Heteroatomic Core-Hole States as a Probe for Nearly Indistinguishable Chemical Environments
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.
Journal of Physical Chemistry Letters
Nascimento, D., Zhang, Y., Bergmann, U., & Govind, N. (2020). Near-Edge X-ray Absorption Fine Structure Spectroscopy of Heteroatomic Core-Hole States as a Probe for Nearly Indistinguishable Chemical Environments. Journal of Physical Chemistry Letters, 11 (2), 556-561. https://doi.org/10.1021/acs.jpclett.9b03500