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.
@article{arxiv.0811.0147,
title = {Coherent State Preparation and Observation of Rabi Oscillations in a Single Molecule},
author = {Ilja Gerhardt and Gert Wrigge and Gert Zumofen and Jaesuk Hwang and Alois Renn and Vahid Sandoghdar},
journal= {arXiv preprint arXiv:0811.0147},
year = {2009}
}