Femtosecond photodesorption of small molecules from surfaces: a theoretical investigation from first principles.
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.
Koch
Christiane P
CP
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany. koch_c@fhi-berlin.mpg.de
Klüner
Thorsten
T
Freund
Hans-Joachim
HJ
Kosloff
Ronnie
R