Photoinduced dynamics of CO on Ru(0001): Understanding experiments by simulations with all degrees of freedom

Mladineo, Bruno; Juaristi, J. Iñaki; Alducin, Maite; Saalfrank, Peter; Lončarić, Ivor (2025) Photoinduced dynamics of CO on Ru(0001): Understanding experiments by simulations with all degrees of freedom. The Journal of Chemical Physics, 163 (4). ISSN 0021-9606

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Abstract

Real-time pump–probe experiments are powerful tools for monitoring chemical reactions but often need parallel theoretical modeling to disentangle different contributions. Monitoring x-ray spectra of photoinduced dynamics of CO on Ru(0001) provided a strong indication for a transient “precursor state” of unidentified nature to various subsequent outcomes. So far, the precise nature of the postulated precursor has also remained elusive in state-of-the-art ab initio molecular dynamics models, including single-moving CO molecules. In the present work, we have constructed a density functional theory-based machine learning interatomic potential energy surface that is valid for all ionic degrees of freedom of the system, comprising many molecules at various coverages and moving surface atoms. Our Langevin dynamics with electronic friction based on the new potential energy surface identified the precursor state as dynamically trapped molecules around 6 Å from the surface that arise from adsorbate–adsorbate interactions. We have compared our results to experimental observations and calculated the dependence of reaction probabilities on pump laser fluence and initial surface coverage.

Item Type:	Article
Uncontrolled Keywords:	machine learning interatomic potential; density functional theory; molecular dynamics
Subjects:	NATURAL SCIENCES > Physics NATURAL SCIENCES > Physics > Condensed Matter Physics
Divisions:	Theoretical Physics Division
Projects:	Project title Project leader Project code Project type Povećanje prostorne i vremenske skale modeliranja materijala iz prvih principa pomoću strojnog učenja-ExtMatModelML Ivor Lončarić UIP-2020-02-5675 HRZZ
Depositing User:	Ivor Lončarić
Date Deposited:	23 Jul 2025 07:03
URI:	http://fulir.irb.hr/id/eprint/9913
DOI:	10.1063/5.0278850

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