Abstract
The selective and nonselective excitations of laser-stimulated surface processes are quantitatively discussed by the population dynamics of multi-photon-multi-phonon processes. The multi-level system is reduced to a few-level system in the Heisenberg-Markovian picture and the level populations of different normal modes of the adspecies/surface system are solved numerically. It is shown that specific normal modes of the system may be selectively excited without appreciably heating the system as a whole when the pumping rate is faster than the energy relaxation rate. In contrast to a homogeneous gas-phase system (governed by picosecond phenomena), much longer time scales of the relaxation dynamics are discussed for the present heterogeneous system.
Published Version
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