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Physical Review A

All-optical scheme for strongly enhanced production of a Bose-Einstein condensate of dipolar molecules in the vibronic ground state

Matt Mackie, Catherine DeBrosse

Published Apr 26, 2010• 1 citation
Publisher

Abstract

We consider two-color heteronuclear photoassociation of a dual-species Bose-Einstein condensate into a Bose-Einstein condensate of dipolar molecules in the $J=1$ 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.

DOI
10.1103/physreva.81.043627

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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.
We consider two-color heteronuclear photoassociation of atoms into dipolar molecules in the J=1 electro-vibrational 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 excited state creates a second pathway for creating ground state molecules, leading to quantum interference between direct photoassociation and photoassociation via the excited molecular state, as well as a dispersive-like 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 semi-classical size of both molecular states. Despite strong enhancement, coherent conversion to the LiNa electro-vibrational ground state is possible only in a limited regime near the free-bound resonance.
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.
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We consider the formation of cold diatomic molecules in the electronic ground state by photoassociation of atoms of dissimilar species. A combination of two transition pathways from the free colliding pair of atoms to a bound vibrational level of the electronic molecular ground state is envisioned. The first pathway consists of a pump-dump scheme with two time-delayed laser pulses in the near-infrared frequency domain. The pump pulse drives the transition to a bound vibrational level of an excited electronic state, while the dump pulse transfers the population to a bound vibrational level of the electronic ground state. The second pathway takes advantage of the existing permanent dipole moment and employs a single pulse in the far-infrared domain to drive the transition from the unbound atoms directly to a bound vibrational level in the electronic ground state. We show that this scheme offers the possibility to coherently control the photoassociation yield by manipulating the relative phase and timing of the pulses. The photoassociation mechanism is illustrated for the formation of cold LiCs molecules.
We investigate theoretically the molecular yield in photoassociation of Bose-Einstein condensed sodium atoms for light intensities of the order of and above those applied in a recent experiment. Our results show that the rate at which ground-state molecules may be formed saturates at high light intensities whereas the loss rate of condensate atoms does not. This is caused by the opposing roles of the short- and long-range pair correlations present near resonance under the influence of the laser and is crucial for the development of efficient photoassociation procedures in a condensate.
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.