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  • Letter
  • Open Access

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

Raúl Bombín1,2,3,*, A. S. Muzas2, Dino Novko4, J. Iñaki Juaristi1,2,5,†, and Maite Alducin2,5,‡

  • 1Departamento de Polímeros y Materiales Avanzados: Física, Química y Tecnología, Facultad de Químicas (UPV/EHU), Apartado 1072, E-20080 Donostia-San Sebastián, Spain
  • 2Centro de Física de Materiales CFM/MPC (CSIC-UPV/EHU), Paseo Manuel de Lardizabal 5, E-20018 Donostia-San Sebastián, Spain
  • 3Departament de Física, Universitat Politècnica de Catalunya, Campus Nord B4-B5, E-08034 Barcelona, Spain
  • 4Institute of Physics, Bijenička 46, HR-10000 Zagreb, Croatia
  • 5Donostia International Physics Center (DIPC), Paseo Manuel de Lardizabal 4, E-20018 Donostia-San Sebastián, Spain

  • *raul.bombin@ehu.eus
  • †josebainaki.juaristi@ehu.eus
  • ‡maite.alducin@ehu.eus
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Phys. Rev. B 107, L121404 – Published 10 March, 2023

DOI: https://doi.org/10.1103/PhysRevB.107.L121404

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 adsorbate nonadiabatic 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 nonequilibrium 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 the dynamics at multicomponent surfaces involving localized and standard s or p states.

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Phys. Rev. B 107, L121404– Published 10 March, 2023
  • Received 15 November 2022
  • Revised 13 February 2023
  • Accepted 1 March 2023
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