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Conference on Lasers and Electro-Optics

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

Ilja Gerhardt, G. Wrigge, Jaesuk Hwang, G. Zumofen, Alois Renn, Vahid Sandoghdar

Published Jan 1, 2009• 6 citations
Publisher

Abstract

We report the observation of up to 5 Rabi cycles in a single molecule. A π-pulse excitation is achieved with 500 photons, marking an important step towards preparation of coherent superposition states with few photons.
DOI
10.1364/iqec.2009.ithh1

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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 $\ensuremath{\pi}$-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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Abstract A single organic dye molecule at cryogenic conditions is resonantly excited in a confocal microscope. Under strong laser illumination it undergoes Rabi oscillations. Mathematically, this was well described and had been experimentally implemented. These oscillations can be measured as side-bands on their resonance fluorescence, e.g. in the Mollow-Triplet. An alternative method is to research this effect by an analysis of the single molecule anti-bunched photon statistics. This has been performed in this work. Here we research on the detuning dependence of this signal—it is experimentally demanding since the utilized laser might drift or single emitters are not necessarily spectrally stable enough, such that the spectrum can be measured indefinitely. We therefore apply a measurement technique in which the photon correlation signal is acquired in detuning dependent steps. This is performed by continuous laser sweeps over the single molecule excitation spectrum. A single recording of the anti-bunched photons takes 20–50 ms. After approx. 1 h of repetitive laser detunings a full anti-bunching curve is reconstructed for each spectral position. An alternative technique with 100 ns laser pulses allows us to acquire a set of comparable data. Our study is derived from a single dibenzanthanthrene molecule with a natural linewidth of 2π×16 MHz. It emits under resonant excitation more than 380.000 photons per second. Under spectral detuning, Rabi-oscillations are observed up to Ω Rabi = 2π×160 MHz.