Ultracold heteronuclear polar KRb molecules have enjoyed tremendous attention for many years now. The presence of a large molecule fixed dipole moment in the absolute rovibrational ground state (v''=0, J'' =0) makes external control very convenient, which opens up the prospect of studying various physical phenomenon in many areas of physics and chemistry. The methods used so far to produce the absolute ground state of KRb have involved very complicated techniques. Molecules formed in weakly bound levels were transferred to the absolute ground state through the multiple steps of transfer processes involving several lasers with extremely narrow linewidths. My thesis research demonstrates an alternate simpler method of formation of the lowest vibrational levels of the ground state utilizing PA combined with radiative decay, which has been so far useful to form ultracold molecules in the higher vibrational levels of the ground state. This thesis presents two main topics of research. The first part of the thesis consists of results describing the scheme which provides a single-step, continuous, and irreversible method of forming KRb molecules in their absolute ground state. The second topic involves spectroscopy on the two excited electronic states of KRb which may provide alternative pathways for the formation of the absolute ground state (X 1Σ+, (v''=0, J'' =0)) and suitable pathways for efficient formation of the lowest metastable state (a 3Σ+, (v''=0, N'' =0)). I believe this research will lay the foundation for many new exciting experiments in the future.
Ultracold heteronuclear polar KRb molecules have enjoyed tremendous attention for many years now. The presence of a large molecule fixed dipole moment in the absolute rovibrational ground state (v''=0, J'' =0) makes external control very convenient, which opens up the prospect of studying various physical phenomenon in many areas of physics and chemistry. The methods used so far to produce the absolute ground state of KRb have involved very complicated techniques. Molecules formed in weakly bound levels were transferred to the absolute ground state through the multiple steps of transfer processes involving several lasers with extremely narrow linewidths. My thesis research demonstrates an alternate simpler method of formation of the lowest vibrational levels of the ground state utilizing PA combined with radiative decay, which has been so far useful to form ultracold molecules in the higher vibrational levels of the ground state. This thesis presents two main topics of research. The first part of the thesis consists of results describing the scheme which provides a single-step, continuous, and irreversible method of forming KRb molecules in their absolute ground state. The second topic involves spectroscopy on the two excited electronic states of KRb which may provide alternative pathways for the formation of the absolute ground state (X 1Σ+, (v''=0, J'' =0)) and suitable pathways for efficient formation of the lowest metastable state (a 3Σ+, (v''=0, N'' =0)). I believe this research will lay the foundation for many new exciting experiments in the future.
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. ^
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. ^
Ultracold atomic gases have proven to be a versatile tool for the study of many-body quantum physics thanks to the high degree of control that they offer. However, interactions between neutral atoms are usually short-ranged and isotropic, which limits their applicability as a simulator of real condensed matter systems. One of the most common methods of introducing stronger interactions into an ultracold gas is associating pairs of atoms of two different elements into molecules. Such molecules possess a body-fixed electric dipole moment, which can be addressed by an external electric field or microwave radiation to engineer long-ranged, tunable dipolar interactions. In addition to constituting an analogue quantum simulator, ultracold dipolar molecules show potential as a platform for digital quantum computation, precision measurements, and the study of quantum chemistry. The main result presented in this thesis is the first successful synthesis of ultracold 39K133Cs molecules in their vibrational and rotational ground state. Using a novel simultaneous cooling scheme for potassium and caesium, our team has been able to produce mixtures that are cold enough for efficient magnetoassociation into weakly bound molecules to take place. By performing high-resolution laser spectroscopy of these molecules, I have identified a two-photon pathway to the ground state via an exceptionally narrow intermediate excited state. I was then able to perform Stimulated Raman Adiabatic Passage (STIRAP) along that pathway with one-way efficiencies up to 71%, producing trapped samples of up to 3500 ground-state molecules at temperatures of 1 µK. The lifetime of these samples is currently limited by a near-universal two-body loss process, a further study of which could shed light on similar loss mechanisms in other molecular species. I have also carried out preliminary rotational spectroscopy, which paves the way towards using KCs molecules as a controlled interacting spin system and a refinement of their hyperfine coupling constants. The thesis ends with a detailed outline of further steps that should be taken to improve the efficiency of STIRAP, as well as the population and coherence lifetimes in KCs samples. It is followed by a list of suggested experiments that could be carried out using our system after it undergoes the described technical upgrades. Some of these experiments are directly inspired by the results I have obtained during my six-month research stay in the KRb laboratory at JILA.
In the first part of this dissertation we develop and successfully demonstrate two methods, based on photoassociation of ultracold potassium atoms, for producing ultracold K2 molecules, with sub mK temperatures, in deeply bound vibrational levels of the ground XS+g 1 state. The principal objective has been to develop an “ultracold molecule factory” that can be used to support experiments on spectroscopy, collisions, and chemistry of ultracold molecules. ^ In the first experiment the ground-state molecules are produced by the radiative decay of excited, n≅191 AS+u 1 state molecules, photoassociated from ultracold potassium atoms in a vapor-cell MOT. The decay is primarily into the vibrational continuum, but a small fraction decays into bound levels of the X state near n = 36. The experimentally observed molecule production rate is about 103 per second. ^ In our second experiment, we use two-step laser excitation to effect an “R-transfer” from long-range to intermediate internuclear separations, greatly increasing the efficiency for radiative production of low- n molecules in the X state. Molecules are formed in the Pg1 state by photoassociation, then excited by a second laser to the 51Pu or 61Pu Rydberg states, in selected vibrational levels from n = 13–18. Finally, radiative decay produces very large numbers of X state molecules with n≅25 and significant numbers of molecules in very low vibrational levels, including n = 0. We have observed production rates up to about 105 molecules/second per vibrational level. ^ In both experiments the ground-state molecules are detected with a sensitive and selective resonant two-color photoionization with nanosecond pulses. ^ In the second part of this dissertation we demonstrate a novel method for high sensitivity absorption measurements, that combines a phase modulated, high-resolution pulsed laser with an actively stabilized optical cavity to achieve a sensitivity of ∼10−9 per cm. This is comparable to the best existing methods for pulsed absorption measurements, but unlike most other methods, it can also be readily extended to the UV region and to Doppler-free spectroscopy. ^
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.
Abstract Heteronuclear alkali-metal dimers represent the class of molecules of choice for creating samples of ultracold molecules exhibiting an intrinsic large permanent electric dipole moment. Among them, the KCs molecule, with a permanent dipole moment of 1.92 Debye still remains to be observed in ultracold conditions. Based on spectroscopic studies available in the literature completed by accurate quantum chemistry calculations, we propose several optical coherent schemes to create ultracold bosonic and fermionic KCs molecules in their absolute rovibrational ground level, starting from a weakly bound level of their electronic ground state manifold. The processes rely on the existence of convenient electronically excited states allowing an efficient stimulated Raman adiabatic transfer of the level population.