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Updated: Jan 8, 2026

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
Published on: August 6, 2018
Multimode vibrational activation and energy transfer in single-molecule CO hopping on Pd(111)
Maki Inagaki1, Minhui Lee1,2, Tae Gyun Kim3
1Surface and Interface Science Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan.
None:
We report a vibrationally induced single-molecule hopping of carbon monoxide (CO) on Pd(111) by action spectroscopy with a scanning tunneling microscope (STM-AS). The observed hopping yields reveal vibrational thresholds at 96, 124, 142, and 230 meV, which correspond to high-order overtones of the metal-carbon (M-C) stretch mode and the fundamental C-O stretch mode. Morse potential fitting enables quantitative estimation of anharmonicity and supports overtone-driven activation. Comparison with previous studies on Pd(110) shows that the significantly higher reaction yield on Pd(111) arises from enhanced anharmonic coupling between high-frequency modes and the frustrated translational mode, the reaction coordinate for lateral hopping. This work emphasizes the role of site-dependent anharmonic interactions in energy transfer, with overtone excitations as an available pathway. Our findings offer new insights into multimode vibrational activation mechanisms in surface reactions and highlight a means of manipulating molecular motion at the atomic scale.
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