Laser-Stimulated Vibrational Excitation of an Adspecies Studied by a Generalized Master Equation: Neutral Atomic Hydrogen on Hydrated KCl(001)

摘要

Vibrational energy transfer between an IR laser, a solid surface and an adatom is studied by a generalized master equation which includes memory effects. Numerical problems associated with the temporally delocalized memory kernel are overcome by introducing the isomnesic approximation. Results obtained for time scales ranging from 2 ps to 2 micro s for H(H2O)/KC1(001) show that effective vibrational excitation is possible with low power lasers (1 W/sq cm) in spite of fast phonon relaxation. Detailed time-evolution of the system is seen to differ radically from that predicted by Markovian theories, even for fairly long time scales.