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The laser-induced desorption of CO molecules from a Cu (111) surface is time resolved with 100-fsec resolution. We find the desorption reaction is completed in 325 fsec after the 100-fsec, 2-eV photon energy pump pulse. The only mechanism consistent with this abrupt, efficient (10^18 cm^2) desorption is a novel one: The transient hot substrate electrons (T₄₋₄₂ₓₑ₎₍, ₌₀ₗ3600 K, while T₋₀ₓₓ₈₂₄, ₌₀ₗ160 K) drive ImultipleP electronic excitation-deexcitation cycles of the CO-Cu complex within the vibrational relaxation time. This vibrationally pumps the molecules into desorbing.
Prybyla et al. (Mon,) studied this question.