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arXiv · 2211.12192

Anomalous transient blueshift in the internal stretch mode of CO/Pd(111)

Raúl Bombín·Alberto S. Muzas·Dino Novko·J. Iñaki Juaristi·Maite Alducin
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Abstract

In time-resolved pump-probe vibrational spectroscopy the internal stretch mode of polar molecules is utilized as a key observable to characterize the ultrafast dynamics of adsorbates on surfaces. The adsorbates non-adiabatic intermode couplings are the commonly accepted mechanisms behind the observed transient frequency shifts. Here, we study the CO/Pd(111) system with a robust theoretical framework that includes electron-hole pair excitations and electron-mediated coupling between the vibrational modes. A mechanism is revealed that screens the electron-phonon interaction and originates a blueshift under ultrafast non-equilibrium conditions. The results are explained in terms of the abrupt change in the density of states around the Fermi level, and are instrumental for understanding dynamics at multi-component surfaces involving localized and standard $s$ or $p$ states.

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Raúl Bombín, Alberto S. Muzas, Dino Novko, J. Iñaki Juaristi, Maite Alducin. 2022-11-22. Anomalous transient blueshift in the internal stretch mode of CO/Pd(111). https://doi.org/10.1103/physrevb.107.l121404

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