Utilizing single-photon photoassociation, we have achieved ultracold rubidium molecules with a high number density that provides a new efficient approach toward molecular quantum degeneracy. A new detection mechanism for ultracold molecules utilizing inelastic atom–molecule collision is demonstrated. The resonant coupling effect on the formation of the X 1 Σ + g ground state 85 Rb 2 allows for a sufficient number of more deeply bound ultracold molecules, which induced an additional trap loss and heating of the co-existing atoms owing to the inelastic atom–molecule collision. Therefore, after the photoassociation process, the ultracold molecules can be investigated using the absorption image of the ultracold rubidium atoms mixed with the molecules in a crossed optical dipole trap. The existence of the ultracold molecules was then verified, and the amount of accumulated molecules was measured. This method detects the final produced ultracold molecules, and hence is distinct from the conventional trap loss experiment, which is used to study the association resonance. It is composed of measurements of the time evolution of an atomic cloud and a decay model, by which the number density of the ultracold 85 Rb 2 molecules in the optical trap was estimated to be >5.2 × 10 11 cm −3 .
Utilizing single-photon photoassociation, we have achieved ultracold rubidium molecules with a high number density that provides a new efficient approach toward molecular quantum degeneracy. A new detection mechanism for ultracold molecules utilizing inelastic atom–molecule collision is demonstrated. The resonant coupling effect on the formation of the X 1 Σ + g ground state 85 Rb 2 allows for a sufficient number of more deeply bound ultracold molecules, which induced an additional trap loss and heating of the co-existing atoms owing to the inelastic atom–molecule collision. Therefore, after the photoassociation process, the ultracold molecules can be investigated using the absorption image of the ultracold rubidium atoms mixed with the molecules in a crossed optical dipole trap. The existence of the ultracold molecules was then verified, and the amount of accumulated molecules was measured. This method detects the final produced ultracold molecules, and hence is distinct from the conventional trap loss experiment, which is used to study the association resonance. It is composed of measurements of the time evolution of an atomic cloud and a decay model, by which the number density of the ultracold 85 Rb 2 molecules in the optical trap was estimated to be >5.2 × 10 11 cm −3 .
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. ^
This thesis describes the results of several experiments that studied the photoassociation of an ultracold atomic Rb gas. In the first experiment, we produced ultracold diatomic molecules from an atomic gas via single-color photoassociation. The molecules were detected with resonance-enhanced multiphoton ionization. Trapping of these molecules in a quadrupole magnetic trap, with lifetimes up to 20 seconds, was also demonstrated. In addition, the rate constant for inelastic collisions between the trapped molecules and atoms was determined from measurements of the atomic density dependence of the decay rate of the trapped molecules. In another experiment, stimulated Raman photoassociation of Rb atoms in a Mott insulator state was studied. A Bose-Einstein condensate (BEC) of 87Rb atoms was loaded into a three-dimensional optical lattice formed by the interference pattern of three orthogonal standing wave laser fields. This system constitutes a very good realization of the Bose-Hubbard model, which predicts a quantum phase transition between a superfluid state and a Mott insulator state at a particular lattice height. A time-of-flight imaging method was used to study the state of the atomic gas, and the quantum phase transition was observed at the predicted lattice height. The signature of the phase transition was the disappearance and reappearance of peaks in the image that arose from the interference of atoms originating from different lattice sites. Two coherent laser fields were applied to the gas in its Mott insulating state, and tuned close to a Raman photoassociation resonance, and this resulted in an observable loss of atoms due to the formation of molecules. This transition exhibited a double-peaked spectrum, with one of the peaks arising from photoassociation of atoms in sites containing only two atoms, and the other from sites containing three atoms. Also, the loss of atoms vs. the duration of the Raman photoassociation period was studied, with the lasers tuned to the peak corresponding to two atoms per site. It was found that a central core of the gas, containing about 40 percent of the atoms, exhibited a coherent oscillation between an atomic and molecular quantum gas.
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.
Significant two-body losses are observed in an ultracold gas of 85Rb or 87Rb atoms in a crossed dipole trap implemented with a broadband laser with a wavelength around 1071 nm. Using available spectroscopic data on the excited states of Rb2, as well as accurate computed transition dipole moment functions, we interpret these losses as due to photoassociation of deeply bound levels of the 0u+ coupled states by the trapping laser, followed by spontaneous emission down to bound levels of the Rb2 ground state thus forming ultracold molecules. The observed ratio of 3.3 between the loss rates of 87Rb and 85Rb is well reproduced by the theoretical model.
Abstract Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes in the dark or to laser-free decay pathways. For atom–molecule mixtures, RbCs + Rb and RbCs + Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom–molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.
Production and state-selective detection of ultracold molecular rubidium (85Rb2) in the singlet ground state and the metastable triplet state are described. Ultracold 85Rb2 molecules are produced via photoassociation followed by radiative decay. State-selective detection of high-ν ground-state and metastable-state molecules is carried out by resonant Two-photon ionization (R2PI) with a pulsed laser. The spectra of both the ground singlet and metastable triplet states are investigated. Spectroscopy of several intermediate excited states, some of which are observed for the first time, is also studied. Mixing between excited singlet and triplet states is observed in both the singlet and triplet spectra. A proposal for producing ν = 0 ground-state molecules by utilizing this singlet-triplet mixing is given. Magnetic trapping and filtering of metastable triplet-state molecules is also described, and a scheme for optical trapping of molecules is proposed.^