Molecular spectroscopy is used to probe a quantum degenerate gas of 7Li atoms. Several effects are investigated using both single-color and two-color (Raman) photoassociative spectroscopy. An unusual spectral shift with laser intensity is observed for single-color photoassociation and the intensity dependence agrees with theoretical predictions. Additionally, the prospects for altering the interactions between ground-state atoms is investigated for both the single-color and Raman schemes. The single-color scheme is found to be impractical experimentally (although feasible theoretically) while the Raman scheme may be experimentally feasible as well. The Raman spectra display an interesting lineshape which is found to reflect the rate for inelastic collisions involving ground-state molecules (produced via the Raman process) as well as the attractive mean-field interactions between atoms in the condensate. Under certain circumstances, a dispersive Raman lineshape is observed which may be due to coherence properties of both the condensate and the thermal gas. Additionally, the Raman lineshape appears to reflect the kinetic time scale for thermal atoms to enter the condensate via elastic collisions. The Raman technique is applied to studies of the condensate growth and collapse dynamics caused by attractive interactions between condensate atoms, and enables the first direct observations of this phenomenon.
Molecular spectroscopy is used to probe a quantum degenerate gas of 7Li atoms. Several effects are investigated using both single-color and two-color (Raman) photoassociative spectroscopy. An unusual spectral shift with laser intensity is observed for single-color photoassociation and the intensity dependence agrees with theoretical predictions. Additionally, the prospects for altering the interactions between ground-state atoms is investigated for both the single-color and Raman schemes. The single-color scheme is found to be impractical experimentally (although feasible theoretically) while the Raman scheme may be experimentally feasible as well. The Raman spectra display an interesting lineshape which is found to reflect the rate for inelastic collisions involving ground-state molecules (produced via the Raman process) as well as the attractive mean-field interactions between atoms in the condensate. Under certain circumstances, a dispersive Raman lineshape is observed which may be due to coherence properties of both the condensate and the thermal gas. Additionally, the Raman lineshape appears to reflect the kinetic time scale for thermal atoms to enter the condensate via elastic collisions. The Raman technique is applied to studies of the condensate growth and collapse dynamics caused by attractive interactions between condensate atoms, and enables the first direct observations of this phenomenon.
A light-induced frequency shift is observed in single-photon photoassociative spectra of magnetically trapped, quantum degenerate 7Li. The shift is a manifestation of the coupling between the threshold continuum scattering states and discrete bound levels in the excited-state molecular potential induced by the photoassociation laser. The frequency shift is observed to be linear in the laser intensity with a measured proportionality constant that is in good agreement with theoretical predictions. This phenomenon has important implications for a scheme to alter the interactions between atoms in a Bose-Einstein condensate using photoassociation resonances.
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.
We study coherent photoassociation, phenomena analogous to coherent optical transients in few-level systems, which may take place in photoassociation of an atomic Bose-Einstein condensate but not in a nondegenerate gas. We develop a second-quantized Hamiltonian to describe photoassociation, and apply the Hamiltonian both in the momentum representation and in the position representation (field theory). The solution of the two-mode problem, including only one mode each for the atomic and molecular condensates, displays analogs of Rabi oscillations and rapid adiabatic passage. A classical version of the field theory for atoms and molecules is used to demonstrate that, in the presence of photoassociating light, a joint atom-molecule condensate is unstable against the growth of density fluctuations. Experimental complications, including spontaneous emission and unwanted ``rogue'' photodissociation from a photoassociated molecule, are analyzed. A two-color Raman scheme is studied as a method to set up an effective two-mode scheme with reduced spontaneous-emission losses. We discuss photoassociation rates and photoassociation Rabi frequencies for high-lying vibrational states in alkali dimers both on the basis of molecular-structure calculations, and by comparing with an experiment [Wynar et al., Science 287, 1016 (2000)].
A dynamical many-body theory of single color photoassociation in a Bose-Einstein condensate is presented. The theory describes the time evolution of a condensed atomic ensemble under the influence of an arbitrarily varying near-resonant laser pulse, which strongly modifies the binary scattering properties. In particular, when considering situations with rapid variations and high light intensities the approach described in this article leads, in a consistent way, beyond standard mean-field techniques. This allows one to address the question of limits to the photoassociation rate due to many-body effects which has caused extensive discussions in the recent past. Both the possible loss rate of condensate atoms and the amount of stable ground-state molecules achievable within a certain time are found to be stronger limited than according to mean-field theory. By systematically treating the dynamics of the connected Green's function for pair correlations the resonantly driven population of the excited molecular state as well as scattering into the continuum of noncondensed atomic states are taken into account. A detailed analysis of the low-energy stationary scattering properties of two atoms modified by the near resonant photoassociation laser, in particular of the dressed state spectrum of the relative motion prepares for the analysis of the many-body dynamics. The consequences of the finite lifetime of the resonantly coupled bound state are discussed in the two-body as well as in the many-body context. Extending the two body description to scattering in a tight trap reveals the modifications to the near resonant adiabatic dressed levels caused by the decay of the excited molecular state.
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.
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.