TY - JOUR

T1 - Coherent state preparation and observation of Rabi oscillations in a single molecule

AU - Gerhardt, I.

AU - Wrigge, G.

AU - Zumofen, G.

AU - Hwang, J.

AU - Renn, A.

AU - Sandoghdar, V.

PY - 2009

Y1 - 2009

N2 - 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 π-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.

AB - 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 π-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.

KW - Dyes

KW - Excited States

KW - Fluorescence

KW - High-speed Optical Techniques

KW - Molecule-photon Collisions

KW - Photoexcitation

KW - Spectral Line Intensity

KW - Spectral Line Shift

U2 - 10.1103/PhysRevA.79.011402

DO - 10.1103/PhysRevA.79.011402

M3 - Article

VL - 79

SP - 011402

JO - Physical Review A

JF - Physical Review A

SN - 2469-9926

IS - 1

ER -