Spectral splitting of a stimulated Raman transition in a single molecule

TL;DR

This paper demonstrates the coherent control of a single molecule's vibrational states via stimulated Raman transition, revealing spectral splitting as a signature, and paves the way for quantum optics applications.

Contribution

It introduces a method to induce and observe stimulated Raman transitions in single molecules, highlighting the spectral splitting as a key signature, with implications for quantum information processing.

Findings

Successful driving of stimulated Raman transition in single molecules

Observation and modeling of spectral splitting as a signature

Potential for applications in quantum optics and information processing

Abstract

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.