Speaker
Description
The internal stretch mode of polar molecules adsorbed on metallic surfaces has emerged as an exceptional test-bed in which to probe many-body theories in current state-of-the-art time-revolved spectroscopy experiments. Here we study non-adiabatic effects on the internal stretch mode of CO adsorbed on the Pd(111) surface by means of first principles calculations [1, 2]. The theoretical
treatment that we employ, including electron-hole pair excitations and electron-mediated coupling between the vibrational modes [3, 4], allows us to study the internal stretch mode under thermal and non-thermal conditions. The latter permits to simulate the conditions that a femtosecond infrared pump pulse generates on the system and to predict the transient red-shift and change in the linewidth
that are induced. The laser-induced non-thermal electron and phonon distributions are described, respectively, by Fermi-Dirac and Bose-Einstein distributions defined by time-dependent electronic Te(t) and lattice Tl(t) temperatures are calculated with a two temperature model (TTM).
[1] R. Bombín, A. S. Muzas, D. Novko, J. I. Juaristi and M. Alducin, Anomalous transient blueshift in the internal stretch mode of CO/Pd(111), Phys. Rev. B 107, L121404 (2023)
[2] R. Bombín, A. S. Muzas, D. Novko, J. I. Juaristi, M. Alducin, Vibrational dynamics of CO on Pd(111) in and out of thermal equilibrium, Phys. Rev. B 108, 045409 (2023)
[3] D. Novko., M. Alducin and J. I. Juaristi, J. I. Juaristi, Electron-Mediated Phonon-Phonon Coupling Drives the Vibrational Relaxation of CO on Cu(100), Phys. Rev. Lett. 120, 156804 (2018).
[4] D. Novko, J. C. Tremblay, M. Alducin, J. I. Juaristi, Ultrafast Transient Dynamics of Adsorbates on Surfaces Deciphered: The Case of CO on Cu(100), Phys. Rev. Lett. 122, 016806 (2018).
