Journal
PHYSICAL REVIEW A
Volume 79, Issue 1, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevA.79.011402
Keywords
dyes; excited states; fluorescence; high-speed optical techniques; molecule-photon collisions; photoexcitation; spectral line intensity; spectral line shift
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Funding
- Schweizerische Nationalfond
- ETH Zurich initiative for Quantum Systems for Information Technology (QSIT)
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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.
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