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arXiv:0804.3011 · Physical Review Letters

Cross-Molecular Coupling in Combined Photoassociation and Feshbach Resonances

Matt Mackie, Matthew Fenty, Danielle Savage, Jake Kesselman

Published Jul 21, 2008• 33 citations
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Abstract

We model combined photoassociation and Feshbach resonances in a Bose-Einstein condensate. When the magnetic field is far-off resonance, cross coupling between the two target molecules--enabled by the shared dissociation continuum--leads to an anomalous dispersive shift in the position of laser resonance, as well as unprecedented elimination and enhancement of resonant photoassociation via quantum interference. For off-resonant lasers, a dispersive shift and quantum interference appear similarly in resonant three-body Feshbach losses, except that the Feshbach node is tunable with intensity.

DOI
10.1103/physrevlett.101.040401

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We model combined photoassociation and Feshbach resonances in a Bose-Einstein condensate. When the magnetic field is far-off resonance, cross coupling between the two target molecules--enabled by the shared dissociation continuum--leads to an anomalous dispersive shift in the position of laser resonance, as well as unprecedented elimination and enhancement of resonant photoassociation via quantum interference. For off-resonant lasers, a dispersive shift and quantum interference appear similarly in resonant three-body Feshbach losses, except that the Feshbach node is tunable with intensity.
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.
We measure the effect of a magnetic Feshbach resonance (FR) on the rate and light-induced frequency shift of a photoassociation resonance in ultracold 7Li. The photoassociation-induced loss-rate coefficient K_{p} depends strongly on magnetic field, varying by more than a factor of 10;{4} for fields near the FR. At sufficiently high laser intensities, K_{p} for a thermal gas decreases with increasing intensity, while saturation is observed for the first time in a Bose-Einstein condensate. The frequency shift is also strongly field dependent and exhibits an anomalous blueshift for fields just below the FR.
The rate of photoassociation (PA) determines how quickly molecules form from atoms illuminated by a resonant laser pulse. Knowledge of limits of this molecular formation rate provide a fundamental component on the maximum rate that a tightly bound ground state molecular Bose-Einstein condensate (BEC) could be formed using a two-photon transition. This molecular synthesis represents the beginning of a new era of ultracold quantum chemistry. The available Feshbach resonance in this system is an indispensable tool to increase the molecular formation rate due to PA in the anticipation of revealing these fundamental rate limits. While the rate saturates in a thermal gas, no evidence of saturation has yet been observed in a BEC. A loss of atoms due to a PA pulse tuned to the v " = 83 excited state molecular vibrational level provides the measurement of the PA rate. The rate varies by several orders of magnitude either by tuning the magnetic field near a Feshbach resonance or by adjusting the PA intensity. We measure the PA rate at magnetic fields between 550-900 Gauss in a BEC and a thermal gas, which is near the Feshbach resonance at 736 Gauss. The rapidly changing rate near the Feshbach resonance reflects the overlap between the ground state and the excited state wavefunctions. We present the first quantitative measurement of the PA rate near a Feshbach resonance. We measure the magnetic field dependence of the molecular resonance position near the Feshbach resonance. We introduce the first observation of a positive energy shift associated with photoassociation. The measured energy shift asymptotically diverges as it approaches the Feshbach resonance and agrees qualitatively with described theory at all magnetic fields. We observe intensity dependent saturation in the PA rate in a thermal gas and the measurements qualitatively agree with a unitarity limited rate. The first conclusive evidence for a suppression of the PA rate occurs for intensities above the saturation intensity. We report the first observed saturation of the PA rate in a BEC. Three separate theories present possible mechanisms for the observed saturation.
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 study the effects of magnetic Feshbach resonance on the shifts in photoassociation (PA) spectra of ultracold Cs atoms. A series of atom loss spectra show a linear variation of the frequency shift with the PA laser intensity at different magnetic fields near the d-wave Feshbach resonance of optically trapped Cs atoms. The magnetic field-dependence of the slope of the shift on the PA laser intensity exhibits a dispersive change near the Feshbach resonance. The theoretical formula derived from a model based on Fano resonance fits well with the experimental data. Using a model rectangular potential with tunable well depth and applying the Franck-Condon principle, we obtain numerical results, which are found to be largely in disagreement with the experimental findings.
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.