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arXiv:quant-ph/0609008 · Physical Review Letters

Precise Control of Molecular Dynamics with a Femtosecond Frequency Comb

Avi Pe’er, Evgeny A. Shapiro, Matthew C. Stowe, Moshe Shapiro, Jun Ye

Published Mar 16, 2007• 81 citations
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Abstract

We present a general and highly efficient scheme for performing narrow-band Raman transitions between molecular vibrational levels using a coherent train of weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulses permits an analytic description within the framework of coherent control in the perturbative regime, while coherent accumulation of many pulse pairs enables near unity transfer efficiency with a high spectral selectivity, thus forming a powerful combination of pump-dump control schemes and the precision of the frequency comb. Simulations verify the feasibility and robustness of this concept, with the aim to form deeply bound, ultracold molecules.

DOI
10.1103/physrevlett.98.113004

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We present a general and highly efficient scheme for performing narrow-band Raman transitions between molecular vibrational levels using a coherent train of weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulses permits an analytic description within the framework of coherent control in the perturbative regime, while coherent accumulation of many pulse pairs enables near unity transfer efficiency with a high spectral selectivity, thus forming a powerful combination of pump-dump control schemes and the precision of the frequency comb. Simulations verify the feasibility and robustness of this concept, with the aim to form deeply bound, ultracold molecules.
An excitation scheme is proposed for transferring population between ground-vibrational levels of a molecule. The transfer is accomplished by pumping and dumping population with a pair of coherent ultrashort-pulse trains via a stationary state. By mismatching the teeth of the frequency combs associated with the pulse trains to the vibrational levels, high selectivity in the excitation, along with high transfer efficiency, is predicted. The pump-dump scheme does not suffer from spontaneous emission losses, it is insensitive to the pump-dump-train delay, and it requires only basic pulse shaping.
We show that a single femtosecond optical frequency comb may be used to induce two-photon transitions between molecular vibrational levels to form ultracold molecules (e.g., KRb). The phase across an individual pulse in the pulse train is sinusoidally modulated with a carefully chosen modulation amplitude and frequency. Piecewise adiabatic population transfer is fulfilled to the final state by each pulse in the applied pulse train, providing a controlled population accumulation in the final state. Detuning the pulse train carrier and modulation frequency from one-photon resonances changes the time scale of molecular dynamics but leads to the same complete population transfer to the ultracold state. A standard optical frequency comb with no modulation is shown to induce similar dynamics, leading to rovibrational cooling.
Abstract A single femtosecond optical frequency comb is implemented to induce two‐photon transitions between molecular vibrational levels to form ultracold molecules. The phase across an individual pulse in the pulse train is sinusoidally modulated with a carefully chosen modulation amplitude and frequency. Piecewise population transfer is fulfilled to the final state by each pulse in the applied pulse train providing a controlled population accumulation in the final, ultracold state. The dynamics of rovibrational cooling is discussed on an example of the KRb molecule. © 2010 Wiley Periodicals, Inc. Int J Quantum Chem, 2010
In this paper, I discuss the selective and efficient vibrational population transfer between electronic states of diatomic molecules by a weak, ultrashort pulse train. The spectrum of each individual pulse in the train is wide enough to simultaneously excite several vibrational levels of the molecule. However, selectivity is achieved by mismatching the frequency comb, associated with the pulse train, to the excited vibrational levels. Efficiency results from the coherent accumulation of population from one pulse in the train to the next.
We propose an improved photoassociation scheme to produce ultracold molecules in their vibronic ground state for the generic case in which nonadiabatic effects facilitating transfer to deeply bound levels are absent. Formation of molecules is achieved by short laser pulses in a Raman-like pump-dump process where an additional near-infrared laser field couples the excited state to an auxiliary state. The coupling due to the additional field effectively changes the shape of the excited-state potential and allows for efficient population transfer to low-lying vibrational levels of the electronic ground state. Repetition of many pump-dump sequences together with collisional relaxation allows for accumulation of molecules in v=0v=0v=0.
We propose a mechanism to produce a superposition of atomic and molecular states by a train of ultrashort laser pulses combined with weak control fields. By adjusting the repetition rate of the pump pulses and the intensity of the coupling laser, one can suppress a transition while simultaneously enhancing the desired transitions. As an example, various superpositions of vibrational states of the K2{\mathrm{K}}_{2}K2​ molecule are shown.