Direct time-domain observation of ultrafast dephasing in adsorbate-substrate vibration under the influence of a hot electron bath: Cs adatoms on Pt(111)

The stretching vibration of Cs adsorbed on Pt(111) is excited coherently by resonant stimulated Raman excitation and its time evolution is probed by fs time-resolved second harmonic generation as a function of pump laser fluence I. As I increases, a fast dephasing component with the lifetime of tau=0.7 ps grows, being superimposed on a slow one with tau=1.9 ps. The fast component is a manifestation of pure dephasing caused by elastic and inelastic scattering of hot electrons at adsorbate.