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Frontiers in Optics

Photoassociation Spectroscopy of Ultracold Atoms and the Study of “Physicist’s Molecules,” a review

K. M. Jones, Eite Tiesinga, Paul D. Lett, Paul S. Julienne

Published Jan 1, 2006• 0 citations
Publisher

Abstract

Photoassociation is the process where two colliding atoms absorb a photon to form molecule. When the initial gas sample is <1mK the technique achieves “atomic” spectral resolution permitting one to extract atomic and molecular properties.
DOI
10.1364/ls.2006.ltue1

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Photoassociation is the process in which two colliding atoms absorb a photon to form an excited molecule. The development of laser-cooling techniques for producing gases at ultracold (<1mK)(<1\phantom{\rule{0.3em}{0ex}}\mathrm{mK})(<1mK) temperatures allows photoassociation spectroscopy to be performed with very high spectral resolution. Of particular interest is the investigation of molecular states whose properties can be related, with high precision, to the properties of their constituent atoms with the ``complications'' of chemical binding accounted for by a few parameters. These include bound long-range or purely long-range vibrational states in which two atoms spend most or all of their time at large internuclear separations. Low-energy atomic scattering states also share this characteristic. Photoassociation techniques have made important contributions to the study of all of these. This review describes what is special about photoassociation spectroscopy at ultracold temperatures, how it is performed, and a sampling of results including the determination of scattering lengths, their control via optical Feshbach resonances, precision determinations of atomic lifetimes from molecular spectra, limits on photoassociation rates in a Bose-Einstein condensate, and briefly, production of cold molecules. Discussions are illustrated with examples on alkali-metal atoms as well as other species. Progress in the field is already past the point where this review can be exhaustive, but an introduction is provided on the capabilities of photoassociation spectroscopy and the techniques presently in use.
Photoassociation reaction is the process in which two colliding atoms (or the colliding atom-molecule system) absorb a photon to form an excited molecule. Since the researches based on the ultracold atomic and molecular systems have attracted great attention both from theorists and experimentalists, the ultracold photoassociation reaction is becoming an ascendant research field. In this paper, we review briefly the investigation history of the photoassociation reaction for ultracold atoms, especially the basic theory of collision and the photoassociation in different light fields, and the research on the external-field manipulation of ultracold atoms collisions is also prospected.
Advances in laser cooling of neutral atoms have made possible a new form of high-resolution laser spectroscopy: photoassociation of ultracold atoms. Colliding neutral atoms, confined in a laser trap, are photoassociated to bound excited states of the dimer molecule by absorbing a photon from a tunable laser. The technique can probe long range and “purely long range” molecular states that are difficult or impossible to detect by traditional means and, because of the extremely low energy of the colliding atoms (<1 mK), is capable of high resolution (<0.001 cm-1). The spectra are useful for atomic lifetime measurements, determination of atomic ground-state scattering information, and measurement of curve-crossing probabilities. Theoretical and experimental work in the field, including multiple resonance techniques and photo association line shapes, are reviewed.
With the ultracold temperatures (T 1012 cm-3) of atoms that can be produced with laser-cooling and trapping techniques, it is now possible to carry out a new kind of high-resolution spectroscopy.1 This photoassociation is based on optical absorption resonances between the initially free states of colliding atoms and specific, bound excited molecular states. High resolution can be obtained because of the narrow energy distribution of the ultracold gas.1 Because the initial states are formed by collisions, it becomes possible to probe unique, excited molecular states with very large interatomic separations that are impossible to probe with conventional molecular spectroscopy. The feasibility of this new spectroscopy has been demonstrated in two recent experiments.2,3
Advances in laser cooling of neutral atoms have made possible a new form of high resolution spectoscopy: photoassociation of ultracold atoms. Colliding neutral atoms, confined in a laser trap, are photoassociated to bound excited states of the dimer molecule by absorbing a photon from a tunable laser. The technique can probe long range and {open_quote}purely long range{close_quote} molecular states that are difficult or impossible to detect by traditional means and, because of the extremely low energy of the colliding atoms (1 mK), is capable of high resolution (0.001 cm{minus}1). Recent results include, the first direct (and most precise) measurement of a molecular dissociation limit, the first observation of retardation effects in atom-atom interactions, high precision measurements of atomic lifetimes, and the study of exotic states of alkali dimers.
In the molecular photoassociation process, two free cold atoms absorb one photon by a resonant way, to create an excited molecule in a well defined ro-vibrational state. The photoassociative spectroscopy of alkaline dimers yields accurate determinations for the long-range parts of molecular potential curves correlated to the first s + p asymptote. In contrast to atoms, laser cooling of molecules is very difficult because of the lack of a closed two-level scheme for recycling the population. The molecular photoassociation of cold atoms opens also a promising alternative for the formation of cold ground state molecules. Photoassociation of cold cesium atoms has permitted the first observation of translationally cold ground state molecules. The case of the cesium atom is very favorable because the 0 g - and 1 u purely long-range states below the dissociation limit 6s 1/2 +6p 3/2 present Condon points at intermediate distances. Such configurations offer rather efficient channels for the creation of singlet or triplet ground state Cs 2 molecules after spontaneous decay.