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New Journal of Physics

Stimulated deceleration of diatomic molecules on multiple rovibrational transitions with coherent pulse trains

Ekaterina Ilinova, Jonathan D. Weinstein, Andrei Derevianko

Published May 6, 2015• 7 citations
Publisher

Abstract

We propose a method of stimulated laser decelerating of diatomic molecules by counter-propagating π -trains of ultrashort laser pulses. The decelerating cycles occur on the rovibrational transitions inside the same ground electronic manifold, thus avoiding the common problem of radiative branching in Doppler cooling of molecules. By matching the frequency comb spectrum of the pulse trains to the spectrum of the R -branch rovibrational transitions we show that stimulated deceleration can be carried out on several rovibrational transitions simultaneously. This enables an increase in the number of cooled molecules with only a single laser source. The exerted optical force does not rely on the decay rates in a system and can be orders of magnitude larger than the typical values of scattering force obtained in conventional Doppler laser cooling schemes.

DOI
10.1088/1367-2630/17/5/055003

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We propose a method of stimulated laser decelerating of diatomic molecules by counter-propagating π -trains of ultrashort laser pulses. The decelerating cycles occur on the rovibrational transitions inside the same ground electronic manifold, thus avoiding the common problem of radiative branching in Doppler cooling of molecules. By matching the frequency comb spectrum of the pulse trains to the spectrum of the R -branch rovibrational transitions we show that stimulated deceleration can be carried out on several rovibrational transitions simultaneously. This enables an increase in the number of cooled molecules with only a single laser source. The exerted optical force does not rely on the decay rates in a system and can be orders of magnitude larger than the typical values of scattering force obtained in conventional Doppler laser cooling schemes.
We propose a method of stimulated laser cooling of diatomic molecules by counter-propagating πππ-trains of ultrashort laser pulses. The cooling cycles occur on the rovibrational transitions inside the same ground electronic manifold, thus avoiding the common problem of radiative branching in Doppler cooling of molecules. By matching the frequency comb spectrum of the pulse trains to spectrum of the R-branch rovibrational transitions we show that stimulated cooling can be carried out on several rovibrational transitions simultaneously, thereby increasing number of cooled molecules. The exerted optical force does not rely on the decay rates in a system and can be orders of magnitude larger than the typical values of scattering force obtained in conventional Doppler laser cooling schemes.
We explore the possibility of decelerating and Doppler cooling an ensemble of two-level atoms by a coherent train of short, nonoverlapping laser pulses. We derive analytical expressions for mechanical force exerted by the train. In frequency space the force pattern reflects the underlying frequency comb structure. The pattern depends strongly on the ratio of the atomic lifetime to the repetition time between the pulses and pulse area. For example, in the limit of short lifetimes, the frequency-space peaks of the optical force wash out. We propose to tune the carrier-envelope offset frequency to follow the Doppler-shifted detuning as atoms decelerate; this leads to compression of atomic velocity distribution about comb teeth and results in a ``velocity comb''---a series of narrow equidistant peaks in the velocity space.
We study Doppler cooling of atoms using a frequency comb and develop a theory to quantitatively describe the process by investigating the interaction of two-level atoms with two counterpropagating pulse trains. We derive the radiative force on atoms and show that each comb mode effectively acts as a cooling laser, thereby indicating that simultaneous laser cooling in multiple cooling channels can be achieved using a single-frequency comb source. Possible experimental applications involving alkali-metal atoms are illustrated.
We consider decelerating and cooling an ensemble of multilevel atoms and molecules with a coherent train of ultrashort laser pulses. In the frequency domain such trains form frequency combs. We propose a novel see-saw scheme of Doppler cooling of multilevel atoms and molecules. In this scheme the teeth of the frequency comb are periodically moved in and out of resonance with the allowed transitions. The see-saw cooling may be carried out in practice by switching carrier-envelope phase offset between predefined values. We study the performance of the see-saw scheme for the simplest prototype three-level ΛΛΛ system and demonstrate its advantage. For these systems we demonstrate a procedure for determining optimal train parameters, and see-saw switching period. We also illustrate the performance of the protocol by numerically simulating time evolution of velocity distribution.
Cold and ultracold molecules are highly desirable for a diverse range of applications in physics and chemistry such as precision measurements, tests of fundamental physics, quantum simulation and information processing, quantum chemistry, and the physics of strongly correlated quantum matter. Laser cooling is usually infeasible in molecules because their rotational and vibrational transitions make is difficult to come up with a closed scattering cycle. Recently, a narrow range of diatomic molecules, one of which is CaF, has been shown to possess a convenient electronic structure and a highly-diagonal Franck-Condon matrix and thus be amenable to laser cooling. This thesis describes experiments on laser cooling of CaF radicals produced in a supersonic source. We first investigate the increased fluorescence when multi-frequency resonant light excites the molecules from the four hyperfine levels of the ground X²∑+(N = 1, v = 0) state to the first excited A²π½ (J’ = 1=2; v’ = 0) state. The number of photons scattered per molecule increases significantly from one or two in the single frequency case to more than 50 before the molecules get pumped into the X²∑+(N = 1; v = 1) state. We demonstrate laser cooling and slowing of CaF using counter-propagating laser light which causes the molecules to scatter more than a thousand photons on the X (N = 1, v = 0, 1) <->A (J’ = 1=2; v’ = 0) transition. The effect of the laser cooling is to slow a group of molecules from 600 ms-1 to about 580 ms-1 and to narrow their velocity distribution from an initial temperature of 3 K down to 300 mK. In addition, chirping the frequency of the cooling light to keep it on resonance with the decelerating molecules doubles the deceleration and further compresses the velocity distribution. The effect of the laser cooling is limited by the optical pumping of molecules in the X (N = 1, v = 2) state.
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.