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Physical Review Letters

Photoassociation spectrum of ultracold Rb atoms

Joseph D. Miller, Robert A. Cline, Daniel J. Heinzen

Published Oct 4, 1993• 240 citations
Publisher

Abstract

We study the photoassociative collisional loss of laser-cooled Rb atoms from a far-off resonance optical dipole force atom trap. We obtain a well-resolved photoassociation spectrum from 50 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ to 980 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ below the first excited dissociation limit of the ${\mathrm{Rb}}_{2}$ molecule. Two vibrational series associated with excited ${\mathrm{Rb}}_{2}$ $^{3}\mathrm{\ensuremath{\Sigma}}_{\mathit{g}}^{+}$ states are clearly visible. Oscillations in the associated Franck-Condon factors reflect the structure of the triplet ground state wave function. Our results clearly demonstrate the potential of photoassociation spectroscopy as a new probe of molecular structure.

DOI
10.1103/physrevlett.71.2204

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Bulletin of the American Physical Society•May 1, 1993•0 citations
We study the photoassociative collisional loss of laser-cooled Rb atoms from a far-off resonance optical dipole force atom trap. We obtain a well-resolved photoassociation spectrum from 50 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1 to 980 cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1 below the first excited dissociation limit of the Rb2{\mathrm{Rb}}_{2}Rb2​ molecule. Two vibrational series associated with excited Rb2{\mathrm{Rb}}_{2}Rb2​ 3\ensuremathΣg+^{3}\mathrm{\ensuremath{\Sigma}}_{\mathit{g}}^{+}3\ensuremathΣg+​ states are clearly visible. Oscillations in the associated Franck-Condon factors reflect the structure of the triplet ground state wave function. Our results clearly demonstrate the potential of photoassociation spectroscopy as a new probe of molecular structure.
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.
The field of laser cooling and trapping of atoms has had a profound impact on many areas of atomic, molecular and optical science. In particular, ultracold atoms colliding in magneto-optical traps typically have relative kinetic energies of 300muK(sim7MHz)300\\mu K (\\sim 7 MHz)300muK(sim7MHz), so free-bound absorption lines are as sharp as bound-bound lines. Moreover, because of very long range centrifugal barriers, only a few collisional partial waves are important (Jprimeprime=0,1J^{\\prime\\prime} = 0, 1Jprimeprime=0,1 and 2 in our work on 39K^{39}K39K). Such photoassociative free-bound absorption allows observation of ``pure long-range molecule'' states (Re=28R_{e} = 28Re​=28 and 39 {\\AA} in 39K2^{39}K_{2}39K2​) as well as long-range levels of known short range states with outer classical turning points of sim20−250AA\\sim 20 - 250 {\\AA}sim20−250AA. Such spectra have been observed by ``trap loss'' (decrease in atomic fluorescence), molecular ionization, and fragment ionization. Optical-optical double resonance (OODR), e.g. through the ``Franck-Condon windows'' of the ``pure long-range'' states, produces readily assignable spectra at higher asymptotes as well. Further extensions of ultracold photoassociative spectroscopy and applications to determination of long range potentials, atomic properties, and Bose-Einstein condensate stability will be presented.
We have produced ultracold polar RbCs molecules via photoassociation starting from laser-cooled 85 Rb and 133 Cs atoms in a dual-species, forced dark magneto-optical trap. The formed electronically excited RbCs* molecules correlated to the Rb(5S 1/2 ) + Cs(6P 1/2 ) dissociation limit are observed by trap loss spectroscopy. Following the decay of these excited RbCs* molecules, the formed ground state molecules are directly ionized by a two-photon single-color pulse dye laser, which is a new ionization mechanism for ground state RbCs molecules and thence detected by time-of-flight mass spectroscopy.
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.
PHOTOASSOCIATION SPECTROSCOPY OF 85Rb2{^{85}}Rb_{2}85Rb2​ NEAR ITS DISSOCIATION LIMIT
We present results which probe the structure of 85Rb2{^{85}}Rb_{2}85Rb2​ very near its lowest dissociation limit. To obtain these results, we used two different variations of photoassociation spectroscopy of laser-cooled and trapped 85Rb{^{85}}Rb85Rb atoms. First, we have determined the positions of twelve of the highest vibrational levels of 85Rb2{^{85}}Rb_{2}85Rb2​, all bound by less than 0.7cm−10.7 cm^{-1}0.7cm−1, with two-color (free-bound-bound) photoassociation spectroscopy. The levels lie in an energy range for which singlet and triplet states are strongly mixed by the hyperfine interaction. We found that we could accurately describe these states with a novel coupled-channels inverse perturbation analysis. In a second experiment, we have carried out Zeeman-resolved photoassociation spectroscopy. This technique allowed us to probe the energy range in the lowest part of the electronic ground state continuum, which lies between the dissociation limits corresponding to different hyperfine states of the separated atoms. With this method, we have observed a Feshbach scattering resonance in the continuum for the first time, which we find can be tuned to zero energy with a magnetic field.
We have confined up to 10{sup 4} {sup 85}Rb atoms in an optical dipole force trap operating up to 65 nm from atomic resonance. For detunings greater than 16 nm, we obtained long confinement times, limited only by background gas collisions, without additional cooling. However, for trapping laser tunings between 4 nm and 16 nm to the red of the lowest Rb (D1) resonance, we observed a novel trap loss mechanism which results in much shorter-trap lifetimes. The trap loss rate is very sensitive to the laser wavelength, and exhibits a complex spectrum. This trap loss may arise from a photo-associative collisional process in which an initially free pair of colliding ground state atoms is promoted to a bound molecular excited state. The bound excited molecule could then be lost from the trap by photoionization, or by spontaneous decay to an untrapped ground state. The results of our preliminary experiments and of further experiments to clarify this novel trap loss process will be presented.