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Physical Review A

Optimum conditions for producing Cs2 molecular condensates by stimulated Raman adiabatic passage

Zhifang Feng, Weidong Li, Lirong Wang, Liantuan Xiao, Suotang Jia

Published Oct 21, 2009• 6 citations
Publisher

Abstract

The optimum conditions for producing ${\text{Cs}}_{2}$ molecular condensates from Cs atomic condensates with high transfer efficiency by stimulated Raman adiabatic passage are presented. Under the extended ``two-photon'' resonance condition, including the two-photon process, the mean-field correction, and the tunneling coupling between two upper excited molecular levels, a high and stable conversion efficiency is realized. The high conversion efficiency could be achieved by following two methods under experimentally less demanding conditions (relatively small effective Rabi frequency for pump laser pulse). One is adjusting the detuning difference between two laser pulses for same effective Rabi frequencies with up to 87.2% transfer efficiency. Another one is adjusting the effective Rabi frequency, the detuning of dump laser for given effective Rabi frequency, and the detuning of pump laser with up to 80.7% transfer efficiency.

DOI
10.1103/physreva.80.043620

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The optimum conditions for producing Cs2{\text{Cs}}_{2}Cs2​ molecular condensates from Cs atomic condensates with high transfer efficiency by stimulated Raman adiabatic passage are presented. Under the extended ``two-photon'' resonance condition, including the two-photon process, the mean-field correction, and the tunneling coupling between two upper excited molecular levels, a high and stable conversion efficiency is realized. The high conversion efficiency could be achieved by following two methods under experimentally less demanding conditions (relatively small effective Rabi frequency for pump laser pulse). One is adjusting the detuning difference between two laser pulses for same effective Rabi frequencies with up to 87.2% transfer efficiency. Another one is adjusting the effective Rabi frequency, the detuning of dump laser for given effective Rabi frequency, and the detuning of pump laser with up to 80.7% transfer efficiency.
Due to the inevitability of nonlinear collisions between particles in ultracold atomic condensate experiments, it is of great significance to study the nonlinear effect for producing ultracold molecules from atomic condensates. In this work, we investigate theoretically the nonlinear effect induced by the two-body collision for producing ultracold Cs2 molecules from ultracold atoms by the stimulated Raman adiabatic passage in a tunneling four-level structure. Under the two-photon resonance condition and the coherent population trapping state, the conversion efficiency is influenced significantly by the nonlinear parameter. Meanwhile, the optimized parameter ranges of the resonance tunneling strength at the unstable excited molecular states, the effective Rabi frequencies of the two-laser fields, and the detuning of the pump field for different nonlinear parameters are suggested to obtain the high conversion efficiency of Cs2 molecules at the ground state. Finally, a maximum conversion efficiency of up to 88.56% can be realized in the optimized parameter ranges.
The process of stimulated Raman adiabatic passage (STIRAP) provides a possible route for the generation of a coherent molecular Bose-Einstein condensate (BEC) from an atomic BEC. We analyze this process in a three-dimensional mean-field theory, including atom-atom interactions and nonresonant intermediate levels. We find that the process is feasible, but at larger Rabi frequencies than anticipated from a crude single-mode lossless analysis, due to two-photon dephasing caused by the atomic interactions. We then identify optimal strategies in STIRAP allowing one to maintain high conversion efficiencies with smaller Rabi frequencies and under experimentally less demanding conditions.
Summary form only given. Coherent conversion of an atomic to a molecular Bose-Einstein condensate (BEC) is a first step towards 'superchemistry', which is the atom optics analog of frequency conversion in nonlinear optics. A number of studies of this have shown that direct conversion via Raman photo-association appears feasible, based on stimulated free-bound and bound-bound transitions in the presence of two laser fields E/sup (1)/=E/sub 0//sup (1)/ cos(/spl omega//sup (1)/t) and E/sup (2)/=E/sub 0//sup (2)/ cos(/spl omega//sup (2)/t). Here pairs of atoms from the two-atom continuum are transferred-via an excited bound molecular state-to a bound molecular state of lower energy. Raman photo-association allows coupling to a single molecular state, which can be selected by the Raman laser frequencies /spl omega//sup (1)/ and /spl omega//sup (2)/. However, practical calculations using available lasers and transitions indicate that coherent transfer is often limited by spontaneous emission from the intermediate molecular excited electronic state. A possible route towards minimizing losses and decoherence from spontaneous emission is to use the stimulated Raman adiabatic passage (STIRAP) method (Drummond et al, Phys. Rev. Lett. vol. 81, p. 3055, 1998) in which a counter-intuitive pulse sequence is used where the first input pulse couples the molecular levels, even when there are no molecules present.
We study two-photon Raman photoassociation for creating a coherent molecular Bose-Einstein condensate (BEC) from an atomic BEC. By exploring the dynamics of the coupled system, we show that the atom-to-molecule conversion efficiency can be controlled by changing the atom-molecule coupling strength and the effective two-photon Raman detuning. Atom-molecule coupling strength and the effective two-photon Raman detuning can be controlled by changing the laser intensity. We analyze the dynamics of the coupled atom-molecular condensate system by changing the laser intensity over a broad range, keeping the effective two-photon Raman detuning fixed. The effective two-photon Raman detuning depends on the two-photon detuning, Rabi frequencies, and the light shifting (AC Stark shift) of the levels. To keep the effective two-photon Raman detuning fixed, the two-photon detuning is varied to compensate for the light shifting of levels with laser intensity. The corresponding changes in the effective decay rates and the scattering length due to the change in the Rabi frequencies have been taken into account. Dependence of the conversion efficiency on the effective two-photon Raman detuning has also been studied by varying the laser intensity over a narrow range, keeping the two-photon detuning unchanged. The dynamics of the coupled system has been studied in Gross-Pitaevskii and modified Gross-Pitaevskii approaches to demonstrate the effect of the higher order nonlinearity (Lee-Huang-Yang term) with the increase in the laser intensity.
The technique of stimulated Raman adiabatic passage (STIRAP) is a highly efficient tool for coherent population transfer in a chainwise-connected three-state quantum system. It is widely accepted that the two-photon resonance between the two end states of the chain is a crucial condition for STIRAP. This assumption is indeed correct when the two driving fields, pump and Stokes, produce nearly equal couplings for their respective transitions. We show analytically, supported by numeric examples, that when the pump and Stokes couplings differ significantly, the two-photon population transfer profile is distorted and its center is shifted away from the two-photon resonance; hence, the optimal operation of STIRAP demands a two-photon detuning. We derive simple analytic estimates for the center and the width of the two-photon profile. The results are of potential importance in situations when the pump and Stokes fields are of different physical natures (e.g., laser and cavity fields) or when two-photon resonance is unwanted (e.g., in the presence of residual light).