Abstract
A microscopic model for the excitation and relaxation processes in photochemistry at surfaces is developed. Our study is based on ab initio calculations and the surrogate Hamiltonian method treating surface electron-hole pairs as a bath of two-level systems. Desorption probabilities and velocities in the experimentally observed range are obtained. The excited state lifetime is calculated, and a dependence of observables on pulse length is predicted.
- Received 22 October 2002
DOI:https://doi.org/10.1103/PhysRevLett.90.117601
©2003 American Physical Society