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arXiv:1108.2303 · Physical Review A

Feshbach-resonant Raman photoassociation in a Bose-Einstein condensate

Matt Mackie, Pierre Phou, Heather J. Boyce, Mannix Shinn, Lev Katz

Published Oct 10, 2011• 7 citations
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Abstract

We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all---regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but stronger ambient inter-atom collisions lead to an unexpected increase in the efficiency of stable molecule production. Numerical results agree reasonably with an analytical approximation.

DOI
10.1103/physreva.84.043614

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We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all---regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but stronger ambient inter-atom collisions lead to an unexpected increase in the efficiency of stable molecule production. Numerical results agree reasonably with an analytical approximation.
Photoassociation and the Feshbach resonance are, in principle, feasible means for creating a molecular Bose-Einstein condensate from an already-quantum-degenerate gas of atoms; however, mean-field shifts and irreversible decay place practical constraints on the efficient delivery of stable molecules using either mechanism alone. We therefore propose Feshbach-stimulated Raman photoproduction, i.e., a combination of magnetic and optical methods, as a means to collectively convert degenerate atoms into a stable molecular condensate with near-unit efficiency.
We consider two-color heteronuclear photoassociation of a dual-species Bose-Einstein condensate into a Bose-Einstein condensate of dipolar molecules in the J=1J=1J=1 vibronic ground state, where a free-ground laser couples atoms directly to the ground state and a free-bound laser couples the atoms to an electronically excited state. This problem raises an interest because heteronuclear photoassociation from atoms to near-ground-state molecules is limited by the small size of the target state. Nevertheless, the addition of the electronically excited state creates a second pathway for creating molecules in the vibronic ground state, leading to quantum interference between direct photoassociation and photoassociation via the excited molecular state, as well as a dispersivelike shift of the free-ground resonance position. Using LiNa as an example, these results are shown to depend on the detuning and intensity of the free-bound laser, as well as the semiclassical size of both molecular states. Whereas strong enhancement enables saturation of the free-ground transition, coherent conversion from a two-species condensate of atoms to a condensate of dipolar molecules in the vibronic ground state is only possible for a limited range of free-bound detunings near resonance.
Although photoassociation and the Feshbach resonance are feasible means in principle for creating a molecular Bose–Einstein condensate (MBEC) from an already quantum-degenerate gas of atoms, collision-induced mean-field shifts and irreversible decay place practical constraints on the efficient Raman delivery of stable molecules. Focusing on stimulated Raman adiabatic passage, we propose that the efficiency of both mechanisms for producing a stable MBEC can be improved by treating the density of the initial atom condensate as an optimization parameter.
We give a brief description of theoretical studies on multi-component systems and detailed discussions on systems with atom-to-molecule conversion. The conversion of two species of atoms into stable molecules through the Feshbach resonance assisted by stimulated Raman adiabatic passage in photoassociation is studied with the help of mean-field Langrange density. The conversion efficiency is large for the fully bosonic system as well as the boson-fermion mixture as long as the general two-photon resonance condition is satisfied.
We theoretically examine Raman photoassociation of a Bose-Einstein condensate, revisiting stimulated Raman adiabatic passage (STIRAP). Due to collisional mean-field shifts, efficient molecular conversion requires strong coupling and low density, either of which can bring about rogue photodissociation to noncondensate modes. We demonstrate explicitly that rogue transitions are negligible for low excited-state fractions and photodissociation that is slower than the STIRAP time scale. Moreover, we derive a reduced-parameter model of collisions, and thereby find that a gain in the molecular conversion efficiency can be obtained by adjusting the atom-atom scattering length with off-resonant magnetoassociation. This gain saturates when the atom-atom scattering length is tuned to a specific fraction of either the molecule-molecule or atom-molecule scattering length. We conclude that a fully optimized STIRAP scheme may offer the best chance for achieving coherent conversion from an atomic to a molecular condensate with photoassociation.
We model combined photoassociation and Feshbach resonances in a Bose-Einstein condensate, where the shared dissociation continuum allows for quantum interference in losses from the condensate, as well as a dispersive-like shift of resonance. A seemingly oversimplified model is revisited, explaining it as based on the limit of weakly bound molecules, reinforcing it with a comparison to numerical experiments that explicitly include dissociation to noncondensate modes, comparing it against the unitarity limit on condensate losses, and lastly, checking its universal implications. In particular, for a resonant laser and an off-resonant magnetic field, these numerical experiments reveal a rate limit on condensate losses that is larger for smaller condensate densities, approaches the rate limit for magnetoassociation alone near the Feshbach resonance, and agrees best with the analytical model for low density. Comparing the analytical rate limit against the unitary limit, which is set by the size of the condensate, agreement is found only for a limited range of near-resonant magnetic fields. Finally, for a resonant magnetic field and an off-resonant laser, the analytical shift of the Feshbach resonance is found to depend on the size of the Feshbach molecule, signifying nonuniversal physics in a strongly interacting system.