Picosecond sum-frequency generation spectroscopy has been employed to study the dynamics of the internal stretch vibration of CO adsorbed on a Si(100) surface. Using the IR pump—sum-frequency generation probe method, the vibrational lifetime of the C–O stretch vibration has been determined to be 2.3±0.5ns. Within the experimental error limits, the identical lifetime was observed for C12O16 and C13O16. No strong dependency on the carrier density in the substrate, inferred from measurements using differently doped crystals, was observed.

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