Theory of Laser-Stimulated Surface Processes. II. A Generalized-Master-Equation Approach to Energy Transfer between an IR Laser, an Adspecies, and Phonons

摘要

The time evolution of the Vibrational states of an adspecies-surface bond (adbond) excited by IR laser radiation and coupled to phonon modes of the solid is obtained by numerical solution of a generalized master equation. For three levels of a system composed of an atom adsorbed at the end of a linear chain, the average adbond energy is seen to have a monotonic and oscillatory component. Under certain resonance conditions, energy is continuously adsorbed by the adbond from both the laser and the phonons. The Markovian approximation is shown to be inappropriate for this case, and a measure of non-Markovian behavior is proposed. Feedback and synergistic effects are discussed.