This thesis presents an experimental apparatus capable of producing and studying ultra-cold mixtures of ⁶Li and Rb, and progress towards the creation of ultra-cold ground state ⁶Li₂ and LiRb molecules. Ultra-cold experiments with molecules have applications in many quantum computation and simulation experiments. We discuss elements of the apparatus which are important to these experiments, including electric field plates in air capable of producing fields up to 18 kV/cm, and a laser system for photoassociation spectroscopy based on two Ti:Sapphire lasers phase locked to the same optical frequency comb. With respect to ⁶Li and ⁸⁵Rb mixtures, we report on the observation of six Feshbach resonances, which represent an important step towards molecule production and future experiments in this heteronuclear mixture. In addition, we demonstrate the production of a BEC of ⁶Li₂ Feshbach molecules, a degenerate Fermi gas of ⁶Li and the formation of BCS pairs. In the ⁶Li system, we report on the high resolution spectroscopy of the v'=20-26 vibrational levels of the c(1³∑⁺g) potential and the v'=29-35 vibrational levels of the A(1¹∑⁺u) potential. In the A(1¹∑⁺u) potential, we find that the v'=31 and v'=35 levels have the largest transition strength and are therefore good candidates to use as intermediate states in molecule formation. We demonstrate atom-molecule dark states in the BEC-BCS crossover regime and additionally use dark-state spectroscopy to make extremely high resolution measurements of the least bound N''=0 ro-vibrational levels in the X(1¹∑⁺g) and a(1³∑⁺u) potential. In addition, we present spectroscopy of all ten N''=0 and N''=2 ro-vibrational levels in the a(1³∑⁺u) potential and furnish a preliminary interpretation of the observed energy structure. Finally, we report on the observation of anomalous Autler-Townes and dark-state spectrum. Using an extension to the standard three level model, we show that these anomalous profiles are due to degeneracies that exist in the bound molecular states, and to the choice of polarization of the coupling fields. These results have a direct impact on molecule formation, and provide a clear guide to future experiments.
This thesis presents an experimental apparatus capable of producing and studying ultra-cold mixtures of ⁶Li and Rb, and progress towards the creation of ultra-cold ground state ⁶Li₂ and LiRb molecules. Ultra-cold experiments with molecules have applications in many quantum computation and simulation experiments. We discuss elements of the apparatus which are important to these experiments, including electric field plates in air capable of producing fields up to 18 kV/cm, and a laser system for photoassociation spectroscopy based on two Ti:Sapphire lasers phase locked to the same optical frequency comb. With respect to ⁶Li and ⁸⁵Rb mixtures, we report on the observation of six Feshbach resonances, which represent an important step towards molecule production and future experiments in this heteronuclear mixture. In addition, we demonstrate the production of a BEC of ⁶Li₂ Feshbach molecules, a degenerate Fermi gas of ⁶Li and the formation of BCS pairs. In the ⁶Li system, we report on the high resolution spectroscopy of the v'=20-26 vibrational levels of the c(1³∑⁺g) potential and the v'=29-35 vibrational levels of the A(1¹∑⁺u) potential. In the A(1¹∑⁺u) potential, we find that the v'=31 and v'=35 levels have the largest transition strength and are therefore good candidates to use as intermediate states in molecule formation. We demonstrate atom-molecule dark states in the BEC-BCS crossover regime and additionally use dark-state spectroscopy to make extremely high resolution measurements of the least bound N''=0 ro-vibrational levels in the X(1¹∑⁺g) and a(1³∑⁺u) potential. In addition, we present spectroscopy of all ten N''=0 and N''=2 ro-vibrational levels in the a(1³∑⁺u) potential and furnish a preliminary interpretation of the observed energy structure. Finally, we report on the observation of anomalous Autler-Townes and dark-state spectrum. Using an extension to the standard three level model, we show that these anomalous profiles are due to degeneracies that exist in the bound molecular states, and to the choice of polarization of the coupling fields. These results have a direct impact on molecule formation, and provide a clear guide to future experiments.
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.
Heteronuclear polar molecules have recently attracted enormous attention owing to their ground state having a large electric dipole moment. The long range anisotropic dipole-dipole interaction in such systems is the basis for a variety of applications including quantum computing, precision measurements, ultracold chemistry and quantum simulations. Heteronuclear bi-alkali molecules, only a small subset of polar molecules, have received special attention mainly because the constituent alkali atoms are easy to laser cool and can be relatively easily associated to form molecules at ultracold temperatures. Our choice, the LiRb molecule, is motivated by the relatively high dipole moment (4.1 Debye) of the LiRb molecule in its rovibronic ground state. In this thesis, we study the LiRb molecule using laser spectroscopy and report, for the first time, the production of ultracold LiRb molecules by photoassociation (PA). The LiRb molecule is the least studied among all bi-alkali molecules and the first spectroscopic measurements on hot vapor phase LiRb molecules were reported only in 2011. We describe these measurements and their significance in chapter 2, after a brief introduction to the field of ultracold polar molecules in chapter 1. In chapter 3, we discuss our apparatus for simultaneous cooling and trapping of Li and Rb atoms in a dual-species magneto-optical trap (MOT) and report the measurement of interspecies collision-induced losses. In chapter 4, we describe the production of ultracold LiRb molecules in excited electronic states by photoassociation (PA). We report the measurements of the C6 coefficients for the Li (2s 2S1/2) + Rb (5p 2P1/2) and the Li (2s 2S1/2) + Rb (5p 2P3/2) asymptotes. We find a molecule formation rate (PLiRb) as high as 3.5x107 s-1 and a PA rate coefficient (KPA) as high as 1.3x10-10 cm3/s, the highest among heteronuclear bi-alkali molecules. In chapter 5, we discuss results on two-photon PA and we conclude, in chapter 6, with a road roadmap of future experiments for the production and detection of ultracold LiRb molecules in their rovibronic ground state.
This thesis describes the spectroscopy work on ultracold 39K 85Rb molecules as part of our effort towards producing ground-state ultracold polar molecules. ^ The starting points of our experiment are laser cooled and trapped K and Rb atoms in dual-species MOTs and the molecule formation method is photoassociation (PA). A fraction of the PA-produced excited-state molecules can spontaneously emit to the two lowest electronic states, the X 1Σ + state and the a 3Σ + state, to form high vibrational level molecules. In order to develop a population transfer scheme to make deeply bound molecules, we have studied the spectroscopy of KRb in several steps. Besides the PA step, we have also carried out a state-selective detection experiment to study the population distribution of the high vibrational level molecules formed via spontaneous emission. The detection method is pulsed-laser based ion time-of-flight mass spectroscopy. Due to the linewidth limitations of the pulsed laser, this detection method can only resolve vibrational structures. A cw laser induced ion depletion spectroscopy technique has been developed in order to obtain rotational resolution. Using this ion depletion method, we have studied a possible stimulated Raman transfer scheme via the 3 1Σ+ state. To this end, we have obtained all the spectroscopic information required to produce deeply bound KRb molecules in a single vibrational and rotational level. ^ Several other spectroscopic studies using the high vibrational level ultracold molecules are also discussed. ^
The production of a quantum gas with strong long - range dipolar interactions is a major scientific goal in the research field of ultracold gases. In their ro - vibrational ground state Li -K dimers possess a large permanent dipole moment, which could possibly be exploited for the realization of such a quantum gas. A production of these molecules can be achieved by the association of Li and K at a Feshbach resonance, followed by a coherent state transfer. In this thesis, detailed theoretical an experimental preparations to achieve state transfer by means of Stimulated Raman Adiabatic Passage (STIRAP) are described. The theoretical preparations focus on the selection of an electronically excited molecular state that is suitable for STIRAP transfer. In this context, molecular transition dipole moments for both transitions involved in STIRAP transfer are predicted for the first time. This is achieved by the calculation of Franck -Condon factors and a determination of the state in which the 6Li - 40K Feshbach molecules are produced. The calculations show that state transfer by use of a single STIRAP sequence is experimentally very well feasible. Further, the optical wavelengths that are needed to address the selected states are calculated. The high accuracy of the data will allow to carry out the molecular spectroscopy in a fast and efficient manner. Further, only a comparatively narrow wavelength tuneability of the spectroscopy lasers is needed. The most suitable Feshbach resonance for the production of 6Li - 40K molecules at experimentally manageable magnetic field strengths is occurring at 155G. Experimentally, this resonance is investigated by means of cross - dimensional relaxation. The application of the technique at various magnetic field strengths in the vicinity of the 155G Feshbach resonance allows a determination of the resonance position and width with so far unreached precision. This reveals the production of molecules on the atomic side of the resonance, thereby establishing the first observation of a many body effect in the crossover regime of a narrow Feshbach resonance. Further, mass dependent factors, with which the equilibration of an induced anisotropic temperature of the trapped particle samples can be described, are experimentally determined for the first time. The type of resonance as well as the measured molecular lifetimes are found to be very well suited for STIRAP transfer. A Raman laser system is designed based on the transition wavelengths and durations of state transfer which are predicted. As the wavelengths of the Raman lasers differ widely but coherence of the light fields is needed, the technical realization of a laser system is challenging. As a part of the laser system, the construction and characterization of a reference optical resonator are presented. Laser frequency stabilization with a linewidth of approximately 500Hz and an Allan deviation below 10−12 for timespans up to several ten seconds are demonstrated. Further, the stabilization of a frequency comb to this reference laser is demonstrated. For the laser spectroscopy of electronically excited Li -K states an interferometric laser frequency stabilization will be used. The device is a commercial design, for which a calibration procedure that enhances the precision by several orders of magnitude is worked out within this thesis. The calibration scheme includes the precise measurement of the stabilization’s wavelength dependent frequency deviations by means of a frequency comb. By the implementation of several calibration steps a remaining frequency deviation of less than 5.7MHz (rms 1.6MHz) in the whole relevant wavelength range 750 - 795 nm is achieved. Only the exceptional precision of the fully calibrated device permits the usage for the Li -K spectroscopy, while the demonstrated wide tuning capability facilitates the completion of the latter in a fast and convenient manner.
The work described in this thesis can be divided into two parts. The first part is concerned with the production of degenerate Fermi gases and Bose-Fermi mixtures. The second part of the thesis describes studies of strongly interacting spin-mixtures of ultracold fermions. We have cooled a magnetically trapped spin-polarized 6Li Fermi gas into quantum degeneracy by sympathetic cooling with bosonic 23Na. In order to do this, we have converted our previously developed apparatus for Bose-Einstein condensation of 23Na into a two-species cooling facility. We have produced 6Li samples with up to 7 × 107 atoms at temperatures below 0.5TF , and up to 3× 107 atoms at temperatures as low as 0.05TF . Further, we have also produced stable quantum degenerate mixtures of 23Na and 6Li, with several million atoms of each species. In a second set of experiments, we have studied strongly interacting spin-mixtures of 6Li. The strength of interactions was resonantly controlled by applying a magnetic field and tuning to “Feshbach resonances”, which occur when the total energy of the colliding particles coincides with the energy of a bound molecular state. These studies are relevant for the continuing quest for a superfluid transition in a Fermi gas. By studying the inelastic decay of the cloud, we have experimentally identified two Feshbach resonances for the inter-state interactions of the two lowest ground states of 6Li. Most importantly, we found that the lifetime of the strongly interacting system is long enough to observe a superfluid transition in the future. The effects of the coherent collisions in 6Li spin-mixtures were studied using radiofrequency (RF) spectroscopy. We demonstrated the absence of mean field “clock shifts” in a two-state mixture of fermions, and have introduced a three-level method to observe the interaction energy shifts. In the strongly interacting regime, near a Feshbach resonance, we have observed universal behavior of the interaction energy, independent of the value of the scattering length. Finally, we have theoretically studied the effects of Pauli blocking during a free expansion of a degenerate Fermi gas. We have concluded that a strongly interacting normal gas will undergo a hydrodynamic expansion even at zero temperature, due to inefficiency of the Pauli suppression of collisions. Therefore, the already observed hydrodynamic expansion cannot be conclusively interpreted as a signature of superfluidity. Thesis Supervisor: Wolfgang Ketterle Title: John D. MacArthur Professor of Physics
The research described in this thesis is part of an international effort with the aim of studying ultracold quantum degenerate gas samples like Bose-Einstein condensates and Fermi degenerate systems, consisting of atoms confined in magnetic or optical traps. The behavior of such samples is governed by the inter-atomic interactions and the resulting properties of the atom-atom scattering. At the relevant temperatures of 1nK to 10µK a key property is the atom-atom scattering length a. In chapter 2 a theoretical method is presented which enables one to describe the interaction and scattering of (ultra)cold atoms to unprecedented precision. It is also unparalleled in comprehensiveness: it allows the prediction of a large and varied set of experimental data for all isotopes of the same element. The method relies on the extraction from experiments of a few (phase) parameters which completely summarize the behavior of the atoms in the (ultra)cold regime. In chapter 3 the method is applied to the "workhorses" of cold-atom physics: the atomic species 85Rb and 87Rb. We extract the foregoing parameters to a very high precision from several recent high precision experiments, allowing us to predict e.g. the 87Rb spinor condensate to be ferromagnetic: a prediction for which the scattering length has to be calculated with a precision better than 1%. We also predict Feshbach resonances at experimentally accessible magnetic field strengths; resonances searched for and found by the experimental group of Rempe. In close collaboration with his group we "fine-tune" the interaction parameters found previously, by making use of only one of the observed resonances. We then obtain agreement with 42 out of the observed 43 resonance field strengths and are able to identify bound states inducing the Feshbach resonances at these locations. Chapter 4 describes the results of this research. With a thorough understanding of the rubidium interactions, we then switch to lithium which has a fermionic (6Li) and a bosonic (7Li) isotope. Both are being used in cold-atom experiments. In chapter 5 we evaluate the interaction parameters for lithium allowing us to predict magnetic field strengths for which a sample of fermionic 6Li atoms can be regarded as strongly interacting. Furthermore, a three-level method for measuring mean-field shifts, based on radio-frequency techniques, is introduced. For weak interactions we find proportionality of resonance shifts to interaction strengths. In the strongly interacting regime, however, these shifts become very small reflecting the quantum unitarity limit and many-body effects. Most interesting is the fact that in this regime the shifts are small both for large positive a and for large negative a, likely reflecting the universality of the interaction energy. In chapters 6 and 7 the interactions between lithium atoms are reinvestigated, making use of newly available experimental data and with the updated interaction parameters special attention is paid to locating field strengths at which magnetically tunable Feshbach resonances occur in the scattering of lithium atoms. In chapter 6 scattering events in a gas of (fermionic) 6Li atoms are studied. In chapter 7 we show that a consistent description of the 6Li+6Li system can be given. We discuss theoretical uncertainties for the position of the wide 6Li Feshbach resonance and present an analytic scattering model for this resonance, based on the inclusion of a field-dependent virtual open-channel state. We predict new Feshbach resonances for the 6Li-7Li system, and their importance for different types of crossover superfluidity models is discussed. Molecules created by magnetically sweeping over these resonances will have a fermionic character. One magnetic field strength is predicted at which two different fermionic molecules can be created simultaneously.