Vibrational energy transfer between surface adsorbates

Research Summary

Vibrational energy transfer between surface coadsorbates may play a crucial role in certain types of reactions, including those involved in heterogeneous catalysis and electrochemical cells. Nevertheless, such energy transfer mechanisms are less well explored than those related to adsorbate-substrate energy transfer. We have chosen CO+D2O coadsorbed on Pt(111) for the study of ultrafast energy transfer among the adsorbates. By using femtosecond infrared-visible sum-frequency generation spectroscopy, we explored the excitation dynamics of CO-Pt frustrated modes and the subsequent energy flow into the D2O overlayers on a picosecond time scale.

fig. 2-1
Ultrafast heat transfer dynamics at CO covered Pt(111) coadsorbed with D2O multilayers.

fig. 2-2
Typical results of time-resolved infrared-visible sum-frequency generation spectroscopy in the region of C-O stretching band. Two peaks are assigned to CO perturbed by coadsorbed D2O (lower frequency) and CO free from D2O (higher frequency), respectively.

References

  • "Ultrafast Vibrational Energy Transfer in the Layers of D2O and CO on Pt(111) Studied with Time-Resolved Sum-Frequency-Generation Spectroscopy",
    M. Nagao, K. Watanabe, and Y. Matsumoto, J. Phys. Chem. C, 113, 11712-11719 (2009).

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