The rate of photoassociation (PA) determines how quickly molecules form from atoms illuminated by a resonant laser pulse. Knowledge of limits of this molecular formation rate provide a fundamental component on the maximum rate that a tightly bound ground state molecular Bose-Einstein condensate (BEC) could be formed using a two-photon transition. This molecular synthesis represents the beginning of a new era of ultracold quantum chemistry. The available Feshbach resonance in this system is an indispensable tool to increase the molecular formation rate due to PA in the anticipation of revealing these fundamental rate limits. While the rate saturates in a thermal gas, no evidence of saturation has yet been observed in a BEC. A loss of atoms due to a PA pulse tuned to the v " = 83 excited state molecular vibrational level provides the measurement of the PA rate. The rate varies by several orders of magnitude either by tuning the magnetic field near a Feshbach resonance or by adjusting the PA intensity. We measure the PA rate at magnetic fields between 550-900 Gauss in a BEC and a thermal gas, which is near the Feshbach resonance at 736 Gauss. The rapidly changing rate near the Feshbach resonance reflects the overlap between the ground state and the excited state wavefunctions. We present the first quantitative measurement of the PA rate near a Feshbach resonance. We measure the magnetic field dependence of the molecular resonance position near the Feshbach resonance. We introduce the first observation of a positive energy shift associated with photoassociation. The measured energy shift asymptotically diverges as it approaches the Feshbach resonance and agrees qualitatively with described theory at all magnetic fields. We observe intensity dependent saturation in the PA rate in a thermal gas and the measurements qualitatively agree with a unitarity limited rate. The first conclusive evidence for a suppression of the PA rate occurs for intensities above the saturation intensity. We report the first observed saturation of the PA rate in a BEC. Three separate theories present possible mechanisms for the observed saturation.
The rate of photoassociation (PA) determines how quickly molecules form from atoms illuminated by a resonant laser pulse. Knowledge of limits of this molecular formation rate provide a fundamental component on the maximum rate that a tightly bound ground state molecular Bose-Einstein condensate (BEC) could be formed using a two-photon transition. This molecular synthesis represents the beginning of a new era of ultracold quantum chemistry. The available Feshbach resonance in this system is an indispensable tool to increase the molecular formation rate due to PA in the anticipation of revealing these fundamental rate limits. While the rate saturates in a thermal gas, no evidence of saturation has yet been observed in a BEC. A loss of atoms due to a PA pulse tuned to the v " = 83 excited state molecular vibrational level provides the measurement of the PA rate. The rate varies by several orders of magnitude either by tuning the magnetic field near a Feshbach resonance or by adjusting the PA intensity. We measure the PA rate at magnetic fields between 550-900 Gauss in a BEC and a thermal gas, which is near the Feshbach resonance at 736 Gauss. The rapidly changing rate near the Feshbach resonance reflects the overlap between the ground state and the excited state wavefunctions. We present the first quantitative measurement of the PA rate near a Feshbach resonance. We measure the magnetic field dependence of the molecular resonance position near the Feshbach resonance. We introduce the first observation of a positive energy shift associated with photoassociation. The measured energy shift asymptotically diverges as it approaches the Feshbach resonance and agrees qualitatively with described theory at all magnetic fields. We observe intensity dependent saturation in the PA rate in a thermal gas and the measurements qualitatively agree with a unitarity limited rate. The first conclusive evidence for a suppression of the PA rate occurs for intensities above the saturation intensity. We report the first observed saturation of the PA rate in a BEC. Three separate theories present possible mechanisms for the observed saturation.
We measure the effect of a magnetic Feshbach resonance (FR) on the rate and light-induced frequency shift of a photoassociation resonance in ultracold 7Li. The photoassociation-induced loss-rate coefficient K_{p} depends strongly on magnetic field, varying by more than a factor of 10;{4} for fields near the FR. At sufficiently high laser intensities, K_{p} for a thermal gas decreases with increasing intensity, while saturation is observed for the first time in a Bose-Einstein condensate. The frequency shift is also strongly field dependent and exhibits an anomalous blueshift for fields just below the FR.
This thesis describes a suite of experimental tools and spectroscopic measurements performed on ultracold ⁶Li molecules. The aim is to create the necessary ingredients for the coherent transfer of the population of ultracold, weakly bound, Feshbach molecules of ⁶Li to deeply bound ro-vibrational levels, making the eventual creation of a Bose-Einstein condensate (BEC) of ground state lithium dimers a reality at the University of British Columbia. Some of the technological milestones include the development of a unique laser system consisting of two Ti:Sapphire lasers frequency stabilized to a femtosecond frequency comb as well as the demonstration of the first in Canada BEC of Feshbach molecules. To determine a suitable path for the coherent transfer using stimulated Raman adiabatic passage (STIRAP) we measure the binding energies of the vibrational levels v''=20-26 of the c(1³Ʃ+g) and v''=29-35 of the A(1¹Ʃ+u) excited states of lithium dimers by the photoassociation of a degenerate Fermi gas of 6Li atoms, achieving accuracy of 600 kHz. For each vibrational level of the triplet potential, we resolve the rotational structure using a Feshbach resonance to enhance the photoassociation rates from p-wave collisions. We also, for the first time, determine the spin-spin and spin-rotation interaction constants for this state. Finally, we are the first to demonstrate exotic dark states in quantum gases of fermionic lithium where atom-molecule coherence is produced between a deeply bound singlet (or triplet) molecular level and atomic pairs in a weakly interacting Fermi gas at zero gauss or in the BEC-BCS crossover regime (i.e. Feshbach molecules or BCS-like pairs). We observe an abrupt and unanticipated change of the classic EIT signature (Electromagnetically Induced Transparency) of the dark-state (i.e. the suppression of single photon absorption to the excited state) in the vicinity of the broad Feshbach resonance at 832.2 gauss potentially indicating new physics not previously considered.
We show how photoassociation (PA) near a magnetically tuned Feshbach resonance can probe the unitarity limit at low laser intensities. This limit occurs when the scattering matrix element in the PA process reaches its quantum limit of one, and is usually difficult to access, requiring large laser intensities. We show how giant enhancements of the PA rate in the vicinity of a Feshbach resonance can reach it, and we predict the appearance of new features with varying magnetic fields and laser intensities. We investigate these effects for a Bose gas of 7 Li atoms at temperatures near quantum degeneracy and give a simple analytical model. We discuss potential applications of our results, obtained without adjustable parameters, to high-precision spectroscopy.
We model combined photoassociation and Feshbach resonances in a Bose-Einstein condensate, where the shared dissociation continuum allows for quantum interference in losses from the condensate, as well as a dispersive-like shift of resonance. A seemingly oversimplified model is revisited, explaining it as based on the limit of weakly bound molecules, reinforcing it with a comparison to numerical experiments that explicitly include dissociation to noncondensate modes, comparing it against the unitarity limit on condensate losses, and lastly, checking its universal implications. In particular, for a resonant laser and an off-resonant magnetic field, these numerical experiments reveal a rate limit on condensate losses that is larger for smaller condensate densities, approaches the rate limit for magnetoassociation alone near the Feshbach resonance, and agrees best with the analytical model for low density. Comparing the analytical rate limit against the unitary limit, which is set by the size of the condensate, agreement is found only for a limited range of near-resonant magnetic fields. Finally, for a resonant magnetic field and an off-resonant laser, the analytical shift of the Feshbach resonance is found to depend on the size of the Feshbach molecule, signifying nonuniversal physics in a strongly interacting system.
An experiment studying the effects of photoassociation in a quantum degenerate gas of 7Li bosons has been performed in a permanent magnet trap. A saturation in the one-photon photoassociation rate and a shift in the resonance due to the applied light field from the 2S 1/2 ground state to the 2P1/2 v ' = 83 excited molecular vibrational state have been measured and compared with theory. Limitations in the ability of the permanent magnet apparatus to study photoassociation in a Bose-Einstein condensate have prompted the development of a magneto-optical trap and an electro-magnetic trap. These new traps will assist in the process of creating a large BEC where the effects of photoassociation will be studied.
This thesis reports on the first observation of optical tuning of interactions in an ultracold atomic gas. To control the elastic interactions, we use optically induced scattering resonances. They are realized by coupling pairs of atoms to a bound molecular state with the help of laser light. In comparison to the well-known magnetic Feshbach resonances, these optical Feshbach resonances allow a very fast switching of interactions in a spatially resolved way. This is because laser light can be switched on and off much faster than magnetic fields and because the light intensity can be spatially structured. Our experiments are performed with a Bose-Einstein condensate (BEC) of Rb atoms, which we produce in our new BEC setup. This apparatus has been constructed in the framework of this thesis and offers excellent optical access to the ultracold atom cloud. To investigate the tunability of atomic interactions with single-frequency laser light, we optically couple pairs of free atoms to an electronically excited molecular state. The coupling is achieved with a laser that is tuned close to the respective free-bound photoassociation transition. By changing the laser detuning we are able to adjust the atomic scattering length to any value between 10 a0 and 190 a0, where a0 denotes the Bohr radius. The atomic scattering length is a single quantity that fully describes ultracold elastic interactions. Since laser induced atom losses restrict the duration of our experiments, Bragg spectroscopy is employed as a fast method to measure the scattering length. We also demonstrate that optical Feshbach resonances can be realized with a two-color Raman coupling scheme. To implement this scheme, a second laser is added that couples the excited molecular state to a weakly bound molecular level in a ground state potential. Tuning the second laser results in a modification of the atomic scattering length similar to the one observed with a single laser. In addition, this scheme allows to control the width of the resonance via the detuning of the first laser. For the one-color and two-color coupling schemes, we investigate how the elastic scattering properties depend on the different available parameters, i.e. the laser detunings and intensities. Our experimental findings can successfully be described with an available theoretical model, which treats ultracold collisions in the presence of laser light. Optical Feshbach resonances have the possibility of becoming a valuable tool for fast switching of interactions. This is of special interest in quantum computation schemes with neutral atoms, where interactions between different atomic qubits need to be controlled.