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O: Fachverband Oberflächenphysik
O 12: Scanning probe microscopy: light matter interaction at atomic scales
O 12.10: Vortrag
Montag, 9. März 2026, 17:15–17:30, HSZ/0403
Tracing vibrational anharmonicity at the submolecular level with tip-enhanced Raman spectroscopy — •Youngwook Park1, Ikutaro Hamada2, Martin Wolf1, and Akitoshi Shiotari1 — 1Fritz-Haber Institute of the Max-Planck Society, Berlin, Germany — 2The University of Osaka, Suita, Japan
Tip-enhanced Raman spectroscopy (TERS) can achieve atomic-scale vibrational imaging, yet overtones and combination bands remain difficult to access due to weak transition strengths. We show that point-contact TERS enables submolecular-resolution detection of intense overtones and combination bands from a single asymmetric perylene derivative on silicon. A 10-times signal increase upon tip–molecule contact allows us to resolve both mechanical and electrical anharmonicities with Å-level spatial contrast. The mapped mechanical anharmonicity reveals a site-specific vibrational energy exchange pathway, demonstrating TERS as a powerful tool for real-space tracking of intramolecular vibrational energy redistribution.
Keywords: Anharmonic coupling; Combination bands; Overtones; Submolecular resolution; TERS