Femtosecond photodesorption of small molecules from surfaces: a theoretical investigation from first principles

Phys Rev Lett. 2003 Mar 21;90(11):117601. doi: 10.1103/PhysRevLett.90.117601. Epub 2003 Mar 17.

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.