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O: Fachverband Oberflächenphysik
O 91: Scanning Probe Microscopy: Light Matter Interaction at Atomic Scales III
O 91.10: Vortrag
Donnerstag, 21. März 2024, 17:30–17:45, MA 041
Resonant TERS of a Single-Molecule Kondo System — •Rodrigo Cezar de Campos Ferreira1, Amandeep Sagwal1,2, Jiří Doležal1,3, Sofia Sofia1, Pablo Merino4, Tomáš Neuman1, and Martin Švec1,5 — 1Institute of Physics, Czech Academy of Sciences; Czech Republic — 2Faculty of Mathematics and Physics, Charles University; Czech Republic — 3Institute of Physics, École Polytechnique Fédérale de Lausanne; Switzerland — 4Instituto de Ciencia de Materiales de Madrid; Spain — 5Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences; Czech Republic
Single-molecule TERS under UHV and cryogenic conditions enables exploration of the relations between the adsorption geometry, electronic state, and vibrational fingerprints[1,2]. Here we precisely lift a PTCDA molecule from a metal surface to bring it into an open-shell spin one-half anionic state. We reveal a correlation between the Kondo resonance in the differential conductance spectroscopy and concurrent characteristic changes captured by the TERS measurements. Through the investigation of various adsorbed and tip-contacted PTCDA scenarios, we infer that the Raman scattering on the suspended PTCDA is resonant with a higher excited state. Theoretical simulation of the vibrational spectra enables a precise assignment of the individual TERS peaks to high-symmetry Ag modes, including the fingerprints of the observed spin state[3]. [1] Y. Zhang et. al. National Science Review, 6, 1169-1175 (2019).[2] R. Jaculbia et. al. Nat. Nanotechnol. 15, 105-110 (2020).[3] R.C.C. Ferreira et. al. arXiv:2310.12546 (2023).
Keywords: TERS; resonant Raman; PTCDA; SPM; break-junction