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Abstract
Quantum state resolved determination of lateral velocity distributions in laser-induced desorption of CO from a Cr2O3(0001) surface is investigated. Experimentally, Doppler profiles are obtained via a (1+1′)-REMPI detection scheme for various rovibrational states and desorption velocities. The experimental findings are directly compared to theoretical results from high-dimensional stochastic quantum dynamical wave packet calculations based on complete first-principles potential energy surfaces. Reasonable quantitative agreement between experiment and theory concerning the total width as well as the full width at half maximum of the lateral velocity distributions is found. Depending on the rotational state a single-peaked or a double-peaked shape of the Doppler profiles is predicted theoretically. In order to support our theoretical predictions we suggest refined experimental investigations of the state-resolved Doppler profiles with an enhanced signal to noise ratio and further theoretical studies concerning the nature of the electronically excited intermediate.
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