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Journal of Physics B Atomic Molecular and Optical Physics

Two-colour photoassociation spectroscopy of ultracold sodium

K. M. Jones, S. Maleki, L. P. Ratliff, Paul D. Lett

Published Jan 28, 1997• 44 citations
Publisher

Abstract

We demonstrate a number of two-colour spectroscopy techniques where the first step is the photoassociation of laser-cooled and trapped sodium atoms to form bound states of . High-resolution spectra of are obtained. Spectra of the `purely long-range' state demonstrates the use of two-colour spectroscopy to open up an ionization channel for detecting the occurrence of photoassociation. The utility of photoassociation as a technique for producing cold molecular samples in a well defined rovibrational state is demonstrated with spectra showing and (Condon internal diffraction) transitions after the photoassociation. Starting from states in the and potentials, these transitions include upward transitions to autoionizing potentials dissociating near 3P + 3P and downward transitions back to the 3S + 3S ground-state potentials. Spectroscopic constants for six levels of a doubly excited state of are given.

DOI
10.1088/0953-4075/30/2/021

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We demonstrate a number of two-colour spectroscopy techniques where the first step is the photoassociation of laser-cooled and trapped sodium atoms to form bound states of . High-resolution spectra of are obtained. Spectra of the `purely long-range' state demonstrates the use of two-colour spectroscopy to open up an ionization channel for detecting the occurrence of photoassociation. The utility of photoassociation as a technique for producing cold molecular samples in a well defined rovibrational state is demonstrated with spectra showing and (Condon internal diffraction) transitions after the photoassociation. Starting from states in the and potentials, these transitions include upward transitions to autoionizing potentials dissociating near 3P + 3P and downward transitions back to the 3S + 3S ground-state potentials. Spectroscopic constants for six levels of a doubly excited state of are given.
We have performed photoassociation spectroscopy to study the doubly excited states of Na2{\mathrm{Na}}_{2}Na2​ involved in the associative ionization of colliding Na(3P)\mathrm{Na}(3P)Na(3P) atoms. Rovibrational levels of two doubly excited potentials connected to the P3/2+P3/2{P}_{3/2}{+P}_{3/2}P3/2​+P3/2​ asymptote, one of ${0}_{u}^{\ensuremath{-}}$ and one of 1u{1}_{u}1u​ symmetry, have been identified. These two doubly excited potentials dominate the route to ionization used in photoassociation experiments of cold Na. Binding energies and rotational constants for all the vibrational levels with binding energies <50GHz<50\mathrm{GHz}<50GHz have been measured. The asymptotic potentials and short-range ionization probabilities are extracted from the data.
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.
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.
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.
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.
We have observed the spectrum of long range molecular states of singly excited Na2{\mathrm{Na}}_{2}Na2​ formed by photoassociation during ultracold associative ionization collisions of laser-cooled Na atoms. The low kinetic energy of the collision allows us to obtain very high resolution spectra and to observe states close to the dissociation limit. The spectrum shows regular vibrational series characteristic of the 1/R3{\mathit{R}}^{3}R3 long range portion of the 1g{1}_{\mathit{g}}1g​ potential (asymptotically S1/2{\mathit{S}}_{1/2}S1/2​+P3/2{\mathit{P}}_{3/2}P3/2​) as well as molecular hyperfine structure within these peaks. We extract potential parameters and compare with recent theory.