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arXiv:1001.3580 · Physical Review A

Achieving ground-state polar molecular condensates by chainwise atom-molecule adiabatic passage

Jing Qian, Weiping Zhang, Hong Yuan Ling

Published Jan 29, 2010• 14 citations
arXivHTMLPDF

Abstract

We generalize the idea of chainwise stimulated Raman adiabatic passage (STIRAP) [Kuznetsova et al., Phys. Rev. A 78, 021402(R) (2008)] to a photoassociation-based chainwise atom-molecule system, with the goal of directly converting two-species atomic Bose-Einstein condensates (BEC) into a ground polar molecular BEC. We pay particular attention to the intermediate Raman laser fields, a control knob inaccessible to the usual three-level model. We find that an appropriate exploration of both the intermediate laser fields and the stability property of the atom-molecule STIRAP can greatly reduce the power demand on the photoassociation laser, a key concern for STIRAPs starting from free atoms due to the small Franck-Condon factor in the free-bound transition.

DOI
10.1103/physreva.81.013632

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We generalize the idea of chainwise stimulated Raman adiabatic passage (STIRAP) [Kuznetsova et al., Phys. Rev. A 78, 021402(R) (2008)] to a photoassociation-based chainwise atom-molecule system, with the goal of directly converting two-species atomic Bose-Einstein condensates (BEC) into a ground polar molecular BEC. We pay particular attention to the intermediate Raman laser fields, a control knob inaccessible to the usual three-level model. We find that an appropriate exploration of both the intermediate laser fields and the stability property of the atom-molecule STIRAP can greatly reduce the power demand on the photoassociation laser, a key concern for STIRAPs starting from free atoms due to the small Franck-Condon factor in the free-bound transition.
Phys. Rev. A 78, 021402(R) (2008)] to a photoassociation-based chainwise atom-moleculesystem, with the goal of directly convertingtwo-species atomic Bose-Einstein condensates(BEC) intoa ground polar molecular BEC. We pay particular attention to the intermediate Raman laser fields,a control knob inaccessible to the usual three-level model. We find that an appropriate explorationof both the intermediate laser fields and the stability property of the atom-molecule STIRAP cangreatly reduce the power demand on the photoassociation laser, a key concern for STIRAPs startingfrom free atoms due to the small Franck-Condon factor in the free-bound transition.
We analyze coherent two-color photoassociation of a Bose-Einstein condensate, focusing on stimulated Raman adiabatic passage (STIRAP) in free-bound-bound transitions from atoms to molecules. This problem raises an interest because STIRAP has been predicted to be absent in the nondegenerate case [Javanainen and Mackie, Phys. Rev. A 58, R789 (1998)]. Nevertheless, we find that Bose stimulation enhances the free-bound dipole matrix element for an atomic condensate, and photoassociative STIRAP turns out to be a viable mechanism for converting an atomic condensate to a molecular condensate with near-unit efficiency.
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.
Collective two-color photoassociation of a freely interacting 87Rb^{87}\mathrm{Rb}87Rb Bose-Einstein condensate is theoretically examined, focusing on stimulated Raman adiabatic passage (STIRAP) from an atomic to a stable molecular condensate. In particular, Drummond et al. [Phys. Rev. A. 65, 063619 (2002)] have predicted that particle-particle interactions can limit the efficiency of collective atom-molecule STIRAP, and that optimizing the laser parameters can partially overcome this limitation. We suggest that the molecular conversion efficiency can be further improved by treating the initial condensate density as an optimization parameter.
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.
We produce 84 Sr 2 molecules using Bose-enhanced Raman photoassociation. We apply the stimulated Raman adiabatic passage (STIRAP) technique on a Bose-Einstein condensate (BEC) to produce more than 8 × 10 3 ultracold molecules. This chemical reaction is only made possible because of the Bose enhancement of the optical transition dipole moment between the initial atomic state and an intermediate molecular state. We study the effect of Bose enhancement by measuring the transition Rabi frequency in a BEC and by comparing it with measurements for two atoms in sites of a Mott insulator. By breaking the dimers' bond and directly observing the separated atoms, we measure the molecular inelastic collision rate parameters. We discuss the possibility of applying Bose-enhanced STIRAP to convert a BEC of atoms into a BEC of molecules, and argue that the required efficiency for STIRAP is within experimental reach.