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arXiv:0801.4796 · Physical Review Letters

Control of Four-Level Quantum Coherence via Discrete Spectral Shaping of an Optical Frequency Comb

Matthew C. Stowe, Avi Pe’er, Jun Ye

Published May 22, 2008• 81 citations
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Abstract

We present experiments demonstrating high-resolution and wide-bandwidth coherent control of a four-level atomic system in a diamond configuration. A femtosecond frequency comb is used to excite a specific pair of two-photon transitions in cold 87Rb. The optical-phase-sensitive response of the closed-loop diamond system is studied by controlling the phase of the comb modes with a pulse shaper. Finally, the pulse shape is optimized resulting in a 256% increase in the two-photon transition rate by forcing constructive interference between the mode pairs detuned from an intermediate resonance.

DOI
10.1103/physrevlett.100.203001

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We present experiments demonstrating high-resolution and wide-bandwidth coherent control of a four-level atomic system in a diamond configuration. A femtosecond frequency comb is used to excite a specific pair of two-photon transitions in cold 87Rb. The optical-phase-sensitive response of the closed-loop diamond system is studied by controlling the phase of the comb modes with a pulse shaper. Finally, the pulse shape is optimized resulting in a 256% increase in the two-photon transition rate by forcing constructive interference between the mode pairs detuned from an intermediate resonance.
A two-photon transition in cold Rb atoms will be probed with a phase-coherent wide bandwidth femtosecond laser comb. Frequency domain analysis yields a high-resolution picture where phase coherence among various transition pathways through different intermediate states produces interference effects on the resonantly enhanced transition probability. This result is supported by the time domain Ramsey interference effect. The two-photon transition spectrum is analyzed in terms of the pulse repetition rate and carrier frequency offset, leading to a cold-atom-based frequency stabilization scheme for both degrees of freedom of the femtosecond laser.
We present experiments demonstrating an enhancement of resonant two-photon transition rate in 87Rb utilizing spectral phase manipulation of the excitation frequency comb. By selectively removing certain comb teeth, the resonant two-photon transition rate can be improved, and reach a factor of more than 1.8. The femtosecond pulse-train excitation of two-photon transition is investigated theoretically based on general multiphoton transitions and the results are compared with the experiments. The theory presented here gives a clear insight of physical mechanism of this quantum coherent control and indicates that it is simple, effective and universal for nonlinear interactions between frequency combs and matters.
We investigate coherent control of the two-photon transition pathways of a four-level atomic system in a diamond configuration. When an ultrashort laser pulse interacts with this system in the ground state 5S1/25{S}_{1/2}5S1/2​ of rubidium, the two-photon transition probability amplitude of 5D3/25{D}_{3/2}5D3/2​ is obtained by a summation of all possible resonant and nonresonant two-photon transition probability amplitudes via 5P1/25{P}_{1/2}5P1/2​ and 5P3/25{P}_{3/2}5P3/2​. Second-order perturbation theory predicts that the maximal constructive interference of the transition probability amplitudes occurs when the phases of eight different spectrum blocks satisfy four different phase relations. Experiments carried out with spectrally phase-coded laser pulses show good agreement with the theoretical prediction.