Abstract
Using resonantly enhanced two-photon ionization, vibrationally excited hydrogen molecules are observed with rotational state selection in associative desorption from a Pd(100) surface. The population in the excited vibrational states of all three stable isotopes is significantly higher than expected for molecules in thermal equilibrium with the surface. Upon changing the surface temperature T s from 325 to 740 K, achieved by employing a permeation source for the hydrogen supply, the vibrational population increases exponentially with T s. A quantum-mechanical approach based on the concept of a reaction-path calculation is applied to this problem. Implications of this model and distinctions from thermal models are discussed.
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