Simulations of x-ray absorption spectra for CO desorbing from Ru(0001) with transition-potential and time-dependent density functional theory approaches

Rodrigues, Gabriel L. S.; Diesen, Elias; Voss, Johannes; Norman, Patrick; Pettersson, Lars G. M.

doi:10.1063/4.0000135

Title: Simulations of x-ray absorption spectra for CO desorbing from Ru(0001) with transition-potential and time-dependent density functional theory approaches

Journal Article · Thu Jan 13 00:00:00 EST 2022 · Structural Dynamics

DOI:https://doi.org/10.1063/4.0000135· OSTI ID:1864595

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^[2]; Voss, Johannes ^[2];

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Stockholm Univ. (Sweden)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
KTH Royal Inst. of Technology, Stockholm (Sweden)

The desorption of a carbon monoxide molecule from a Ru(0001) surface was studied by means of X-ray Absorption Spectra (XAS) computed with Transition Potential (TP-DFT) and Time Dependent (TD-DFT) DFT methods. By unraveling the evolution of the CO electronic structure upon desorption, we observed that at 2.3 Å from the surface, the CO molecule has already predominantly gas-phase character. While C 1s XAS is quite insensitive to changes in the C–O bond length, the O 1s excitation is very sensitive with the π* coming down in energy upon CO bond stretching, which competes with the increase in orbital energy due to the repulsive interaction with the metallic surface. We show in a systematic way that the TP-DFT method can describe the XAS rather well at the endpoints (chemisorbed and gas phase) but is affected by artificial charge transfer and/or incorrect spin treatment in the transition region in cases like CO, where there are low-lying π* orbitals and large exchange interactions between the core 1s and valence-acceptor π* orbitals. As an alternative, we demonstrate by comparing with experimental data that a linear response approach using TD-DFT employing common exchange-correlation functionals and finite-size clusters can yield a good description of the spectral evolution of the 1s → π* transition with correct spin and gas-to-chemisorbed chemical shifts in good agreement with experiment.

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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). Chemical Sciences, Geosciences & Biosciences Division; Knut and Alice Wallenberg Foundation; Swedish National Infrastructure for Computing (SNIC); Swedish Research Council (SRC); USDOE

Contributing Organization:: SUNCAT

Grant/Contract Number:: AC02-76SF00515; KAW2016.0042; 2018–05973; 2018–4343; AC02–05CH11231; FWP 100435

OSTI ID:: 1864595

Alternate ID(s):: OSTI ID: 1839773

Report Number(s):: 100435; KAW-2016.0042; TRN: US2305741

Journal Information:: Structural Dynamics, Vol. 9, Issue 1; ISSN 2329-7778

Publisher:: American Crystallographic Association/AIPCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
X-ray absorption spectroscopy
Surface and interface chemistry
Linear response
Exchange correlation functionals
Exchange interactions
Carbon monoxide
Time dependent density functional theory
Adsorption

Title: Simulations of x-ray absorption spectra for CO desorbing from Ru(0001) with transition-potential and time-dependent density functional theory approaches

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