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Optically driven surface reactions: Evidence for the role of hot electrons.

Evidence is presented for the role of excited conduction electrons in the laser-induced desorption of NO from Pt(111). State-specific detection of the desorbed NO establishes that the rotational distributions are non-Boltzmann, the spin-orbit population is inverted, and that both the translational and vibrational distributions are uncorrelated with the laser-induced surface-temperature jump. The role of optically excited substrate electrons in driving the desorption process is evidenced by a dramatic dependence of the vibrational and translation energy distributions on the desorption-laser wavelengths.