Spectral splitting of a stimulated Raman transition in a single molecule

The small cross section of Raman scattering poses a great challenge for its direct study at the single-molecule level. By exploiting the high Franck-Condon factor of a common-mode resonance, choosing a large vibrational frequency difference in electronic ground and excited states and operation at T...

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Bibliographic Details
Published in:arXiv.org 2023-07
Main Authors: Zirkelbach, Johannes, Gurlek, Burak, Mirzaei, Masoud, Shkarin, Alexey, Utikal, Tobias, Götzinger, Stephan, Sandoghdar, Vahid
Format: Article
Language:English
Subjects:
Coupling (molecular)
Raman spectra
Online Access:Get full text
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Summary:The small cross section of Raman scattering poses a great challenge for its direct study at the single-molecule level. By exploiting the high Franck-Condon factor of a common-mode resonance, choosing a large vibrational frequency difference in electronic ground and excited states and operation at T < 2K, we succeed at driving a coherent stimulated Raman transition in individual molecules. We observe and model a spectral splitting that serves as a characteristic signature of the phenomenon at hand. Our study sets the ground for exploiting the intrinsic optomechanical degrees of freedom of molecules for applications in solid-state quantum optics and information processing.
ISSN:2331-8422
DOI:10.48550/arxiv.2302.14733