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Optical double resonance photoassociation spectrum of ground state Rb_2

R. S. Freeland, Chin‐Chun Tsai, Daniel J. Heinzen, J. M. M. J. Vogels, S. J. J. M. F. Kokkelmans, BOUDEWIJN J. VERHAAR

Published Apr 1, 1997• 0 citations
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Abstract

We report the first observation of the highest lying bound levels of the ground electronic state of ^85Rb2 by means of optical double resonance (free-bound-bound) photoassociation spectroscopy of colliding, laser-cooled ^85Rb atoms. Twelve levels with binding energies from 0.13 to 20 Ghz are observed. We carry out an inverse perturbation analysis of these levels that takes full account of the hyperfine-induced singlet-triplet mixing with a coupled channels approach. This analysis yields previously undetermined atomic interaction parameters that are crucial for the understanding of Rb ultracold collisions and Bose-Einstein condensates. Complete consistency is obtained with all previously measured cold collision properties of Rb. We gratefully acknowledge the support at Texas of the R. A. Welch Foundation, the NSF, and the Microgravity Science and Applications Division of NASA.

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This thesis comprises two topics in the field of the ultracold atomic and molecular physics, both involving formation of ultracold 85Rb 2 by photoassociation (PA). Typically, these ground-state molecules are formed mainly in the very highest vibrational levels, rather than the low-v levels that will be required for most future investigations of ultracold molecular physics and chemistry. The first topic of my research is a method for circumventing this problem: resonant enhancement (RE) of photoassociative ground-state molecule production. The key idea of RE is to photoassociate pairs of colliding atoms into an excited state that has a bimodal vibrational probability distribution, with one peak at long range to enhance the photoassociation rate and another at shorter range to enhance radiative decay into deeply bound levels of the ground state. This can be arranged thanks to the strong spin-orbit perturbative interaction between the two 0+u states converging to two different asymptotes, (5s + 5p1/2) and (5s + 5 p3/2). This method enhances ground-state molecule formation in the region well below the dissociation limit. The experimental work described here was done at the University of Connecticut in collaboration with C. P. Koch at the Institut für Theoretische Physik, Freie Universität Berlin, Germany, who performed the theoretical analysis [1].^ The second part of my thesis is the investigation of ultracold molecules in an optical dipole trap. We have constructed a quasi-electrostratic optical trap (QUEST) for 85Rb using a focused CO2 laser [2]. This provides a very high density of ultracold atoms, up to 10 12 cm-3, providing much higher photoassociation rates. It also keeps the molecules trapped once they have formed. The QUEST provides an ample trapping lifetime for both trapped atoms and molecules, yielding about 4-5×106 atoms and about 9×105 high-v molecules. The long lifetime of the trapped molecules and atoms, combined with their high density, allows us to study interactions such as atom-molecule or molecule-molecule collisions in the ultracold regime. A preliminary experiment on Rb2 molecular decay is described. ^

•Jan 1, 2010•0 citations
We report the first observation of the highest lying bound levels of the ground electronic state of ^85Rb2 by means of optical double resonance (free-bound-bound) photoassociation spectroscopy of colliding, laser-cooled ^85Rb atoms. Twelve levels with binding energies from 0.13 to 20 Ghz are observed. We carry out an inverse perturbation analysis of these levels that takes full account of the hyperfine-induced singlet-triplet mixing with a coupled channels approach. This analysis yields previously undetermined atomic interaction parameters that are crucial for the understanding of Rb ultracold collisions and Bose-Einstein condensates. Complete consistency is obtained with all previously measured cold collision properties of Rb. We gratefully acknowledge the support at Texas of the R. A. Welch Foundation, the NSF, and the Microgravity Science and Applications Division of NASA.
We determine the energies of twelve vibrational levels lying within 20 GHz of the lowest dissociation limit of 85Rb2{}^{85}{\mathrm{Rb}}_{2}85Rb2​ with two-color photoassociation spectroscopy of ultracold 85Rb{}^{85}\mathrm{Rb}85Rb atoms. The levels lie in an energy range for which singlet and triplet states are mixed by the hyperfine interaction. We carry out a coupled channels bound state analysis of the level energies, and derive accurate values for 85Rb2{}^{85}{\mathrm{Rb}}_{2}85Rb2​ interaction parameters. The information obtained is sufficient to allow for quantitative calculations of arbitrary Rb ultracold collision properties.
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 describe a method that is well suited to analysis of the bound states of the alkali-metal dimers near their dissociation limit. The method combines inverse perturbation theory, coupled-channel bound-state theory, and the accumulated phase method to treat the short-range part of the molecular potentials. We apply this method to analyze the bound-state energies measured in a two-color photoassociation experiment in an ultracold 85Rb{}^{85}\mathrm{Rb}85Rb gas. This analysis yields information on the interactions between ultracold 85Rb{}^{85}\mathrm{Rb}85Rb atoms that is important to the understanding of ultracold Rb collisions and Bose-Einstein condensation.
The spectra of the high-lying vibrational levels of the Asp1Sigmasbspu+A\\sp1\\Sigma\\sbsp{u}{+}Asp1Sigmasbspu+ and 1sp3Sigmasbspg+1\\sp3\\Sigma\\sbsp{g}{+}1sp3Sigmasbspg+ singly excited states of both sp6rmLisb2\\sp6\\rm Li\\sb2sp6rmLisb2 and sp7rmLisb2\\sp7\\rm Li\\sb2sp7rmLisb2 are obtained via photoassociation of colliding ultracold atoms confined in a magneto-optical trap. The least bound state of the asp3Sigmasbspu+a\\sp3\\Sigma\\sbsp{u}{+}asp3Sigmasbspu+ ground state potential, obtained by two-photon photoassociative spectroscopy, is also presented for both sp7rmLisb2\\sp7\\rm Li\\sb2sp7rmLisb2 and sp6rmLisb2\\sp6\\rm Li\\sb2sp6rmLisb2. The vibrational levels have resolved hyperfine structure, whose relative energy splittings and transition strengths are accurately modeled. The photoassociative spectra are used to precisely determine both the singlet and triplet s-wave scattering lengths for both isotopes, which are important parameters in systems designed to observe quantum degenerate effects and Bose-Einstein condensation.
We form ultracold ground-state Rb 2 molecules by photoassociating pairs of atoms in a magneto-optical trap into the 0 u + state, which decays radiatively into high vibrational levels of the X 1 Σ g + state. Sensitive and vibrationally state-selective detection is achieved by means of resonantly-enhanced two-photon ionization with a pulsed laser. Frequency scans of the detection laser reveal a long vibrational progression to a previously unobserved electronic excited state, which we identify as the 2 1 Σ u + state. Most of its vibrational spectrum is in excellent agreement with predictions based on ab initio potentials, although the lowest vibrational levels exhibit strong perturbative mixing with the triplet 2 3 Π u state. The detection method reported here, with minor variations, should be effective for the entire potential well of the X state. In this work no transitions are observed from vibrational levels above v = 118, but this turns out to be a limitation not of the detection method but rather of the photoassociative formation scheme, due to re-excitation of the highest- v levels by the same photoassociation laser that produces them.
This thesis comprises two topics in the field of the ultracold atomic and molecular physics, both involving formation of ultracold 85Rb 2 by photoassociation (PA). Typically, these ground-state molecules are formed mainly in the very highest vibrational levels, rather than the low-v levels that will be required for most future investigations of ultracold molecular physics and chemistry. The first topic of my research is a method for circumventing this problem: resonant enhancement (RE) of photoassociative ground-state molecule production. The key idea of RE is to photoassociate pairs of colliding atoms into an excited state that has a bimodal vibrational probability distribution, with one peak at long range to enhance the photoassociation rate and another at shorter range to enhance radiative decay into deeply bound levels of the ground state. This can be arranged thanks to the strong spin-orbit perturbative interaction between the two 0+u states converging to two different asymptotes, (5s + 5p1/2) and (5s + 5 p3/2). This method enhances ground-state molecule formation in the region well below the dissociation limit. The experimental work described here was done at the University of Connecticut in collaboration with C. P. Koch at the Institut für Theoretische Physik, Freie Universität Berlin, Germany, who performed the theoretical analysis [1].^ The second part of my thesis is the investigation of ultracold molecules in an optical dipole trap. We have constructed a quasi-electrostratic optical trap (QUEST) for 85Rb using a focused CO2 laser [2]. This provides a very high density of ultracold atoms, up to 10 12 cm-3, providing much higher photoassociation rates. It also keeps the molecules trapped once they have formed. The QUEST provides an ample trapping lifetime for both trapped atoms and molecules, yielding about 4-5×106 atoms and about 9×105 high-v molecules. The long lifetime of the trapped molecules and atoms, combined with their high density, allows us to study interactions such as atom-molecule or molecule-molecule collisions in the ultracold regime. A preliminary experiment on Rb2 molecular decay is described. ^