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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• Reversible state transfer between light and a single trapped atom
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• Perfect Reflection of Light by an Oscillating Dipole
• Realization of two Fourier-limited solid-state single-photon sources