Nonadiabatic vibrational dynamics of CO on Pt(111) studied with first-principles many-body perturbation theory
Abstract
We investigate the nonequilibrium vibrational dynamics of CO adsorbed on Pt(111), a prototypical adsorbate-surface system for ultrafast vibrational spectroscopy, using a first-principles framework that combines many-body perturbation theory with density functional theory. Within this methodology we explicitly account for electron-hole pair excitations and electron-mediated phonon-phonon coupling. For the latter mechanism, we evaluate the vertex-correction screening, what constitutes a methodological novelty. Our calculations qualitatively reproduce the transient evolution of the internal stretch vibrational mode observed in femtosecond pump-probe experiments, allowing us to identify in the experimental measurements a small transient blueshift after excitation with a femtosecond laser pulse. As predicted in a previous work, the reduction in the number of electronic states available for electron-phonon coupling when the electronic temperature raises at a group 10 transition metal surface, effectively screens the electron-phonon interaction giving rise to an anomalous transient blue-shift.
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BibTeX
@misc{bombin2026nonadiabatic,
title = {{Nonadiabatic vibrational dynamics of CO on Pt(111) studied with first-principles many-body perturbation theory}},
author = {Raúl Bombín and Iñaki Fernández Tena and J. Iñaki Juaristi and Maite Alducin},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.31727},
eprint = {2610.31727},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.31727},
note = {CC BY-NC-SA 4.0},
}
RIS
TY - UNPB
TI - Nonadiabatic vibrational dynamics of CO on Pt(111) studied with first-principles many-body perturbation theory
AU - Raúl Bombín
AU - Iñaki Fernández Tena
AU - J. Iñaki Juaristi
AU - Maite Alducin
PY - 2026
DA - 2026/10/22
PB - arXiv
DO - 10.48550/arxiv.2610.31727
UR - https://arxiv.org/abs/2610.31727
AB - We investigate the nonequilibrium vibrational dynamics of CO adsorbed on Pt(111), a prototypical adsorbate-surface system for ultrafast vibrational spectroscopy, using a first-principles framework that combines many-body perturbation theory with density functional theory. Within this methodology we explicitly account for electron-hole pair excitations and electron-mediated phonon-phonon coupling. For the latter mechanism, we evaluate the vertex-correction screening, what constitutes a methodological novelty. Our calculations qualitatively reproduce the transient evolution of the internal stretch vibrational mode observed in femtosecond pump-probe experiments, allowing us to identify in the experimental measurements a small transient blueshift after excitation with a femtosecond laser pulse. As predicted in a previous work, the reduction in the number of electronic states available for electron-phonon coupling when the electronic temperature raises at a group 10 transition metal surface, effectively screens the electron-phonon interaction giving rise to an anomalous transient blue-shift.
ER -