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The response of the molecular stretch mode of CO/Cu(100) near 2086 cm−1 (ν1) to resonant infrared, and nonresonant visible and ultraviolet pumping is measured on a picosecond time scale. Fourier transform infrared measurements establish that ν1 is anharmonically coupled to the frustrated translation near 32 cm−1 (ν4), so that transient shifts in ν1 indicate population changes in ν4. The ν1 response to visible and ultraviolet pumping is characterized by a spectral shift near zero delay time, which decays with a ≊2 ps time constant to an intermediate value, which then decays on a ≊200 ps time scale. The data agree well with a model whereby ν4 couples to both the photogenerated hot electrons and to the heated phonons. The characteristic coupling times to these two heat baths are found to both be a few picoseconds.
Germer et al. (Fri,) studied this question.