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The small cross section of Raman scattering poses a great challenge for itsdirect study at the single-molecule level. By exploiting the high Franck-Condonfactor of a common-mode resonance, choosing a large vibrational frequencydifference in electronic ground and excited states and operation at T < 2K, wesucceed at driving a coherent stimulated Raman transition in individualmolecules. We observe and model a spectral splitting that serves as acharacteristic signature of the phenomenon at hand. Our study sets the groundfor exploiting the intrinsic optomechanical degrees of freedom of molecules forapplications in solid-state quantum optics and information processing.

Spectral splitting of a stimulated Raman transition in a single molecule