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arXiv:0811.0147 · Physical Review A

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

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

Published Jan 28, 2009• 59 citations
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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 $\ensuremath{\pi}$-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.

DOI
10.1103/physreva.79.011402

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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 \ensuremathπ\ensuremath{\pi}\ensuremathπ-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.
Single molecules in a crystal at low temperature are driven simultaneously by a laser and by the electric field of an rf. At weak rf power, we observe Rabi transitions within doublets of dressed states, the first such observation in condensed matter in the optical domain. At higher rf power, resonances involving several rf photons appear. The interplay between rf and laser dynamics induces shifts and broadenings that are in excellent agreement with calculations from optical Bloch equations. We also directly display the Rabi and multi-rf-photon resonances by recording the fluorescence signal versus the rf frequency.
We present recent results on the coherent control of an optical transition in a single rubidium atom, trapped in an optical tweezer. We excite the atom using resonant light pulses that are short (4 ns) compared with the lifetime of the excited state (26 ns). By varying the intensity of the laser pulses, we can observe an adjustable number of Rabi oscillations, followed by free decay once the light is switched off. To generate the pulses we have developed a novel laser system based on frequency doubling a telecoms laser diode at 1560 nm. By setting the laser intensity to make a pi-pulse, we use this coherent control to make a high quality triggered source of single photons. We obtain an average single photon rate of 9600 s-1 at the detector. Measurements of the second-order temporal correlation function show almost perfect antibunching at zero delay. In addition, we present preliminary results on the use of Raman transitions to couple the two hyperfine levels of the ground state of our trapped atom. This will allow us to prepare and control a qubit formed by two hyperfine sub-levels.
We present recent results on the coherent control of an optical transition in a single rubidium atom, trapped in an optical tweezer. We excite the atom using resonant light pulses that are short (4 ns) compared with the lifetime of the excited state (26 ns). By varying the intensity of the laser pulses, we can observe an adjustable number of Rabi oscillations, followed by free decay once the light is switched off. To generate the pulses we have developed a novel laser system based on frequency doubling a telecoms laser diode at 1560 nm. By setting the laser intensity to make a pi-pulse, we use this coherent control to make a high quality triggered source of single photons. We obtain an average single photon rate of 9600 s-1 at the detector. Measurements of the second-order temporal correlation function show almost perfect antibunching at zero delay. In addition, we present preliminary results on the use of Raman transitions to couple the two hyperfine levels of the ground state of our trapped atom. This will allow us to prepare and control a qubit formed by two hyperfine sub-levels.
Rabi oscillations reflect the existence of a coherent superposition of two molecular eigenstates during the interaction of molecules with a strong, resonant electromagnetic field. This phenomenon is not restricted to two-level systems. We demonstrate its occurrence in a three-level system where the radiation induces a two-photon absorption. The intermediate level is (slightly) detuned from resonance. For a theoretical description the dressed-state picture is adopted. The two-photon excitation is performed either by using one laser, yielding a one-color two-photon process, or by using two counterpropagating, spatially overlapping laser beams, yielding a two-color two-photon process. Rabi oscillations are produced by varying the fluence, i.e., by changing either the laser power or the molecule-laser interaction time. For the one-color case the two-photon transition dipole moment for an SF6{\mathrm{SF}}_{6}SF6​ transition has been determined from the relation between laser fluence and number of Rabi oscillations. For the two-color cases the detuning with the intermediate level is varied by tuning the respective laser frequencies while keeping the sum frequency constant. A dramatic change in the degree of excitation as a function of the intermediate detuning has been observed. \textcopyright{} 1996 The American Physical Society.
We have demonstrated that coherent molecular modulation can result in the collinear generation of mutually-coherent spectral sidebands that extend in frequency from the infrared to the far ultraviolet. Our technique is based on adiabatic preparation of a highly coherent molecular superposition-state, which is achieved by using narrow-linewidth lasers slightly detuned from a Raman resonance. The phases of the resultant Stokes and anti-Stokes sidebands are adjusted in order to synthesize desired single-cycle pulse trains at the target. In this article we review recent improvements and developments in this area, including: techniques for increasing the number of generated sidebands; synchronization of the pulse trains with the molecular motion in the given molecular system; laser self-focusing and spatial soliton formation due to the coherent interaction of light with oscillating molecules. In the future, this Raman source may produce sub-cycle optical pulses, and allow synthesis of waveforms where the electric field is a predetermined function of time, not limited to a quasi-sinusoidal oscillation.