Tip-Enhanced Vibrational Ladder Climbing in Surface Molecular System
Abstract
Achieving high-lying vibrational states is essential for actively controlling molecular reactions. We demonstrate vibrational ladder climbing of CO adsorbed on Pt(111) within the plasmonic tip-substrate nanogap formed in a scanning tunneling microscope, detected via tip-enhanced sum-frequency generation (TE-SFG). As the infrared pulse energy increases, hot-band peaks appear sequentially up to the 3-4 transition, indicating the stepwise population of higher vibrational states. Numerical analysis using the optical Bloch equations captures the observed energy dependence of these features. These results demonstrate the capability of TE-SFG to probe vibrational ladder climbing in surface molecular systems and suggest a promising route toward accessing high-lying vibrational states and controlling vibrational excitation at the nanoscale.
Versions
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BibTeX
@misc{mochizuki2026tipenhanced,
title = {{Tip-Enhanced Vibrational Ladder Climbing in Surface Molecular System}},
author = {Tatsuto Mochizuki and Shota Takahashi and Atsunori Sakurai and Toshiki Sugimoto},
howpublished = {arXiv},
year = {2026},
month = aug,
doi = {10.48550/arxiv.2608.01698},
eprint = {2608.01698},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2608.01698},
}
RIS
TY - UNPB
TI - Tip-Enhanced Vibrational Ladder Climbing in Surface Molecular System
AU - Tatsuto Mochizuki
AU - Shota Takahashi
AU - Atsunori Sakurai
AU - Toshiki Sugimoto
PY - 2026
DA - 2026/08/03
PB - arXiv
DO - 10.48550/arxiv.2608.01698
UR - https://arxiv.org/abs/2608.01698
AB - Achieving high-lying vibrational states is essential for actively controlling molecular reactions. We demonstrate vibrational ladder climbing of CO adsorbed on Pt(111) within the plasmonic tip-substrate nanogap formed in a scanning tunneling microscope, detected via tip-enhanced sum-frequency generation (TE-SFG). As the infrared pulse energy increases, hot-band peaks appear sequentially up to the 3-4 transition, indicating the stepwise population of higher vibrational states. Numerical analysis using the optical Bloch equations captures the observed energy dependence of these features. These results demonstrate the capability of TE-SFG to probe vibrational ladder climbing in surface molecular systems and suggest a promising route toward accessing high-lying vibrational states and controlling vibrational excitation at the nanoscale.
ER -