Coherent State Preparation and Observation of Rabi Oscillations in a Single Molecule

Abstract

We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser intensity, and frequency detuning. A pi-pulse excitation was demonstrated with merely 500 photons, and 5 Rabi cycles were achieved at higher excitation powers. Our findings are in good agreement with theoretical calculations and provide a first step toward coherent manipulation of the electronic states of single molecules with few photons.

4 pages, 3 figures

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• Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence
• Reversible state transfer between light and a single trapped atom
• Strong interaction between light and a single trapped atom without a cavity
• Perfect Reflection of Light by an Oscillating Dipole
• Realization of two Fourier-limited solid-state single-photon sources

Cited by in corpus (8)

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• Coherent Nonlinear Single Molecule Microscopy
• Optical tracing of multiple charges in single-electron devices
• Dissipative stabilization of maximal entanglement between non-identical emitters via two-photon excitation
• Organic molecules as single-photon sources
• Sub-nanosecond coherent optical manipulation of a single aromatic molecule at cryogenic temperature