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arXiv:0806.1295 · Physical Review Letters

Giant Formation Rates of Ultracold Molecules via Feshbach-Optimized Photoassociation

Philippe Pellegrini, Marko Gacesa, Robin Côté

Published Aug 1, 2008• 107 citations
arXivHTMLPDF

Abstract

Ultracold molecules offer a broad variety of applications, ranging from metrology to quantum computing. However, forming "real" ultracold molecules, i.e., in deeply bound levels, is a very difficult proposition. Here, we show how photoassociation in the vicinity of a Feshbach resonance enhances molecular formation rates by several orders of magnitude. We illustrate this effect in heteronuclear systems, and find giant rate coefficients even in deeply bound levels. We also give a simple analytical expression for the photoassociation rate and discuss future applications of the Feshbach-optimized photoassociation technique.

DOI
10.1103/physrevlett.101.053201

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Ultracold molecules offer a broad variety of applications, ranging from metrology to quantum computing. However, forming "real" ultracold molecules, i.e., in deeply bound levels, is a very difficult proposition. Here, we show how photoassociation in the vicinity of a Feshbach resonance enhances molecular formation rates by several orders of magnitude. We illustrate this effect in heteronuclear systems, and find giant rate coefficients even in deeply bound levels. We also give a simple analytical expression for the photoassociation rate and discuss future applications of the Feshbach-optimized photoassociation technique.
Quantum degenerate molecular gases are of interest for the unique level of control they offer over chemical interactions and processes. To reach the quantum degenerate regime, these molecular gases must be cooled to ultracold temperatures, typically on the order of 100 nanoKelvins. Unlike atoms, with a few-level system that facilitates cooling, molecules represent a many-level system, which makes these temperatures experimentally difficult to achieve. As a result, experiments have turned to photoassociation and Feshbach resonance as shortcuts to form ultracold molecules from already ultracold atoms. Photoassociation and Feshbach resonance have been utilized to successfully create stable quantum degenerate molecules, but not on a routine basis, and only for a small range of molecular species. The primary focus of this thesis will be to study photoassociation and Feshbach resonance, and investigate possible routes to more efficient long-lived quantum degenerate molecule formation. We will also investigate realistic limiting conditions to open the possibility to more routine molecules, and to molecular species that are currently inaccessible. Overall, we find combined photoassociation and Feshbach resonance are viable schemes for efficiently creating quantum degenerate molecules, under realistic restrictions such as low laser intensity, narrow Feshbach resonance, and strong elastic collisions. As the techniques to create quantum degenerate molecules become more robust and experimentally available, the creation of colder, larger, and more long-lived samples will facilitate study of these molecules, and spur development into new applications.
Two-color photoassociation of ground state 6{}^{6}6Li87{}^{87}87Rb molecules via the $B\phantom{\rule{0.16em}{0ex}}{}^{1}\ensuremath{\Pi}$ electronic state using short pulses near a magnetic Feshbach resonance is studied theoretically. A near-resonant magnetic field is applied to mix the hyperfine singlet and triplet components of the initial wave function and enhance the photoassociation rate, before the population is transferred to the ground state by a second pulse. We show that an increase of up to three orders of magnitude in the absolute number of molecules produced is attainable for deeply bound vibrational levels. This technique can be generalized to other molecules with accessible magnetic Feshbach resonances.
This review describes recent experimental and theoretical advances in forming molecules in ultracold gases of trapped alkali metal atoms, both by magnetic tuning through Feshbach resonances and by photoassociation. Molecular Bose-Einstein condensation of long-range states of both boson dimers and fermion dimers was achieved in 2002-3. Condensates of boson dimers were found to be short-lived, but long-lived condensates of fermion dimers have been produced. Signatures of triatomic and tetraatomic molecules have recently been observed. Both homonuclear and heteronuclear molecules have been formed by photoassociation, mostly in very high vibrational levels. Recent attempts to produce ultracold molecules in short-range states (low vibrational levels) are described. Experimental and theoretical work on collisions of ultracold molecules is discussed.
We report on the observation of photoassociation resonances in ultracold collisions between ^{23}Na^{40}K molecules and ^{40}K atoms. We perform photoassociation in a long-wavelength optical dipole trap to form deeply bound triatomic molecules in electronically excited states. The atom-molecule Feshbach resonance is used to enhance the free-bound Franck-Condon overlap. The photoassociation into well-defined quantum states of excited triatomic molecules is identified by observing resonantly enhanced loss features. These loss features depend on the polarization of the photoassociation lasers, allowing us to assign rotational quantum numbers. The observation of ultracold atom-molecule photoassociation resonances paves the way toward preparing ground-state triatomic molecules, provides a new high-resolution spectroscopy technique for polyatomic molecules, and is also important to atom-molecule Feshbach resonances.
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We develop the theory for the Adiabatic Raman Photoassociation (ARPA) of ultracold atoms to form ultracold molecules in the presence of scattering resonances. Based on a computational method in which we replace the continuum with a discrete set of "effective modes", we show that the existence of resonances greatly aids in the formation of deeply bound molecular states. We illustrate our general theory by computationally studying the formation of 85^{85}85Rb2_22​ molecules from pairs of colliding ultracold 85^{85}85Rb atoms. The single-event transfer yield is shown to have a near-unity value for wide resonances, while the ensemble-averaged transfer yield is shown to be higher for narrow resonances. The ARPA yields are compared with that of (the experimentally measured) "Feshbach molecule" magneto-association. Our findings suggest that an experimental investigation of ARPA at sub-μμμK temperatures is warranted.