Accuracy of XAS theory for unraveling structural changes of adsorbates: CO on Ni(100)

Diesen, Elias; Rodrigues, Gabriel S.; Luntz, Alan C.; Abild-Pedersen, Frank; Pettersson, Lars G. M.; Voss, Johannes

doi:10.1063/5.0028002

Title: Accuracy of XAS theory for unraveling structural changes of adsorbates: CO on Ni(100)

Journal Article · Wed Nov 11 00:00:00 EST 2020 · AIP Advances

DOI:https://doi.org/10.1063/5.0028002· OSTI ID:1688464

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SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
Stockholm Univ. (Sweden)

Studying surface reactions using ultrafast optical pump and X-ray probe experiments relies on accurate calculations of X-ray spectra of adsorbates for correct identification of the spectral signatures and their dynamical evolution. We show that experimental XAS can be well reproduced for the different binding sites in a static prototype system CO/Ni(100) at a standard DFT (GGA) level of theory, using a plane-wave basis and pseudopotentials. This validates its utility in analyzing ultrafast X-ray probe experiments. The accuracy of computed relative core level binding energies is about 0.2 eV, representing a lower limit for which spectral features can be resolved with this method. We also show that the commonly used Z +1 approximation gives very good core binding energy shifts overall. However, we find a discrepancy for CO adsorbed in the hollow site, which we assign to the significantly stronger hybridization in hollow bonding than in on-top.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Knut and Alice Wallenberg Foundation

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; KAW-2016.0042; FWP 100435

OSTI ID:: 1688464

Alternate ID(s):: OSTI ID: 1712505; OSTI ID: 1769033

Journal Information:: AIP Advances, Vol. 10, Issue 11; ISSN 2158-3226

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

Country of Publication:: United States

Language:: English

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