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AIP conference proceedings

Photoassociative ionization spectroscopy in ultracold sodium

Paul D. Lett, L. P. Ratliff, Mark E. Wagshul, S. L. Rolston, William D. Phillips

Published Jan 1, 1995• 1 citation
Publisher

Abstract

Recent advances in laser cooling techniques have made possible a new type of spectroscopy. In the first experiments of this kind alkali atoms are laser cooled to temperatures around 1 mK and trapped, using laser fields, at densities around 1011 cm−3. Atoms colliding under such ultracold conditions can be resonantly photoassociated to bound states of the dimer molecules. These molecules can in turn be photoionized, providing a sensitive detection of the photoassociation spectrum and revealing in extremely high resolution the structure of the dimer molecules. The particular advantages of this technique include high resolution and signal‐to‐noise and the ability to reach extremely long range states of the molecule, accessible only through such slow collisions.

DOI
10.1063/1.47567

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Recent advances in laser cooling techniques have made possible a new type of spectroscopy. In the first experiments of this kind alkali atoms are laser cooled to temperatures around 1 mK and trapped, using laser fields, at densities around 1011 cm−3. Atoms colliding under such ultracold conditions can be resonantly photoassociated to bound states of the dimer molecules. These molecules can in turn be photoionized, providing a sensitive detection of the photoassociation spectrum and revealing in extremely high resolution the structure of the dimer molecules. The particular advantages of this technique include high resolution and signal‐to‐noise and the ability to reach extremely long range states of the molecule, accessible only through such slow collisions.
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.
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.
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
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.
We present a new spectroscopic technique which allows the observation of long-range molecular states of ultracold sodium via the associative ionization (AI) reaction. Due to the ultracold conditions, we are able to achieve very high resolution spectra of free-bound molecular transitions which were previously observable only via bound-bound spectroscopy. Previous experiments using laser cooled sodium have revealed evidence of molecular spectra but were limited to a narrow tuning range and power broadened because the intense trapping laser was also used to excite the molecular transitions. By alternating the beams of a magneto-optical trap with a separate laser, we confine the atoms while leaving them unperturbed by the trapping light during the excitation period. The second laser excites free ground state atoms into the bound molecular states. With this scheme, we have been able to detect the vibrational series of molecular states in the intermediate AI excitation step, from just below threshold to 3 cm{sup {minus}1} deep. By resolving narrow structure within the spectra associated with molecular hyperfine splittings and comparing with theoretical calculations, we can unambiguously identify the molecular states involved.
The photoassociation of colliding ultracold trapped atoms permits the observation of high resolution molecular spectra of high lying vibrational levels with low total angular momentum and outer turning points greater than 50 Å. This paper describes how the hyperfine structure of alkali dimer molecules at large internuclear separation can be used to assign the electronic character of the observed photoassociation spectra and how hyperfine structure helps to explain the observed photoassociation spectrum of the attractive electronic states of the Na2 molecule that correlate with Na(3 2S)+Na(3 2P3/2) atoms.