Ultracold bialkali polar molecules play a leading part at the frontline of quantum physics. They recently attract a lot of attention in the field of ultracold quantum chemistry, quantum many-body physics and quantum simulations. The key for their success is the rich internal level structure with rotational and vibrational degrees of freedom and their large electric dipole moments. Still, only a handful of molecular species are available at ultracold temperatures until now, although it is highly desirable to produce new molecular species to further expand the range of applications. Besides direct laser cooling methods for molecules, the assembly of heteronuclear ground-state molecules from ultracold atomic mixtures is the most promising approach for the creation of polar molecules. It includes the formation of weakly bound Feshbach molecules from the diatomic mixture and the subsequent two-photon stimulated Raman adiabatic passage (STIRAP) transfer to the rovibrational ground state. This creation strategy has been successfully demonstrated for the first time in the pioneering experiments at JILA with ultracold 40K87Rb molecules. Since then, only a few more molecular species from different alkali atoms have been created, namely 6Li23Na, 23Na40K, 23Na87Rb and 87Rb133Cs. In this thesis, I report the successful creation of a new species of ultracold polar ground-state molecules: 23Na39K. Starting from an ultracold mixture of bosonic 23Na and 39K atoms, weakly bound molecules are created. For this purpose, a Feshbach resonance in a high angular momentum scattering channel is chosen, experimentally identified and characterized. Close to this resonance the weakly bound Feshbach molecules are formed using resonant radio frequency radiation. For the two-photon ground-state transfer, a unique, highly specialized two-color laser system is designed and realized. It is used for one- and two-photon spectroscopy to identify the relevant transitions for the ground-state transfer. Based on the obtained data, a local model of the singlet-triplet mixed excited state manifolds is developed, with which the hyperfine structure and the magnetic field dependence is predicted with high accuracy. According to these findings, a suitable pathway to a single hyperfine ground state is chosen considering selection rules and experimental conditions such as laser polarization and beam alignment. To precisely determine the two-photon resonance condition for STIRAP, electromagnetically induced transparency measurements are performed. The ground-state transfer is then performed using STIRAP. The experimental findings regarding the STIRAP are successfully supported theoretically by a model based on a five-level master equation. The pure molecular gas shows evidence for two-body dominated loss mechanisms, such as sticky four-body collisions. The molecule-atom mixture of 23Na39K+39K reveals an unexpectedly low loss rate coefficient although sticky three-body collisions are assumed to occur. This behavior demands further investigations regarding different hyperfine collisional chan-nels and magnetic field regions.
Ultracold bialkali polar molecules play a leading part at the frontline of quantum physics. They recently attract a lot of attention in the field of ultracold quantum chemistry, quantum many-body physics and quantum simulations. The key for their success is the rich internal level structure with rotational and vibrational degrees of freedom and their large electric dipole moments. Still, only a handful of molecular species are available at ultracold temperatures until now, although it is highly desirable to produce new molecular species to further expand the range of applications. Besides direct laser cooling methods for molecules, the assembly of heteronuclear ground-state molecules from ultracold atomic mixtures is the most promising approach for the creation of polar molecules. It includes the formation of weakly bound Feshbach molecules from the diatomic mixture and the subsequent two-photon stimulated Raman adiabatic passage (STIRAP) transfer to the rovibrational ground state. This creation strategy has been successfully demonstrated for the first time in the pioneering experiments at JILA with ultracold 40K87Rb molecules. Since then, only a few more molecular species from different alkali atoms have been created, namely 6Li23Na, 23Na40K, 23Na87Rb and 87Rb133Cs. In this thesis, I report the successful creation of a new species of ultracold polar ground-state molecules: 23Na39K. Starting from an ultracold mixture of bosonic 23Na and 39K atoms, weakly bound molecules are created. For this purpose, a Feshbach resonance in a high angular momentum scattering channel is chosen, experimentally identified and characterized. Close to this resonance the weakly bound Feshbach molecules are formed using resonant radio frequency radiation. For the two-photon ground-state transfer, a unique, highly specialized two-color laser system is designed and realized. It is used for one- and two-photon spectroscopy to identify the relevant transitions for the ground-state transfer. Based on the obtained data, a local model of the singlet-triplet mixed excited state manifolds is developed, with which the hyperfine structure and the magnetic field dependence is predicted with high accuracy. According to these findings, a suitable pathway to a single hyperfine ground state is chosen considering selection rules and experimental conditions such as laser polarization and beam alignment. To precisely determine the two-photon resonance condition for STIRAP, electromagnetically induced transparency measurements are performed. The ground-state transfer is then performed using STIRAP. The experimental findings regarding the STIRAP are successfully supported theoretically by a model based on a five-level master equation. The pure molecular gas shows evidence for two-body dominated loss mechanisms, such as sticky four-body collisions. The molecule-atom mixture of 23Na39K+39K reveals an unexpectedly low loss rate coefficient although sticky three-body collisions are assumed to occur. This behavior demands further investigations regarding different hyperfine collisional chan-nels and magnetic field regions.
The field of ultracold matter has developed rapidly over the course of the past twenty to thirty years. One outstanding achievement has been the realisation of Bose-Einstein condensation (BEC) only 23 years ago. Many other fascinating observations of quantum phenomena have been made at an incredibly fast pace using ultracold atomic samples with contact force interactions as a testbed. Due to the rapid successes of all these experiments on atomic ensembles, researchers began to aim for more elaborate inter-particle interactions. A possible additional one is the dipole-dipole interaction (DDI), the long-range character of which stands out in comparison to the contact interactions. Moreover, DDI is anisotropic and the possibility to tune the direction of the dipoles in the experiment as well as the interaction strength promises the possibility to study a plethora of new quantum phenomena. In recent years, several experiments using different combinations of alkali atoms to create ground-state hetero-nuclear molecules in the ultracold regime have been set up, following the pioneering work on KRb molecules. Of all possible combinations of two alkali atoms, NaK combines the advantages of a high induced electric dipole moment of 2.72 Debye, chemical stability of the ground-state molecules, the possibility to realise bosonic as well as fermionic molecules and a large knowledge base for cooling and trapping of the two atomic species. This thesis reports on the development and construction of an experiment apparatus for the production of ultracold bosonic dipolar ground state 23Na39K molecules. This includes the setup of an ultra-high vacuum (UHV) system, several laser light sources, microwave (MW) and radio frequency (RF) antennas and electronics to control the various components of the experiment. The system pre-cools the atomic samples of 23Na and 39K and loads them into a dual-species three-dimensional magneto-optical trap (3D MOT). After a transfer to a magnetic quadrupole trap, the mixture is cooled by forced MW evaporation until three-body losses limit dual-species operation at high densities and zero magnetic field. Using the pure optical trapping potential of a crossed optical dipole trap (cODT) and RF- state-transfer, the scattering properties of the bosonic mixture of 23Na+39K are investigated in extensive atom loss measurements for a magnetic field range from 0 to 750 G. Several Feshbach resonances, zero crossings of the interspecies scattering length and inelastic loss features in many different scattering channels are identified. The results of this study are used to refine the molecular potentials of NaK and to produce a dual-species quantum-degenerate mixture of two BECs in the state (f = 1, mf = −1) of 23Na + (f = 1, mf = −1) of 39K. The measurements and refined molecular potentials will considerably aid in the future realisation of 23Na39K molecules in their absolute ground state.
Ultracold quantum gases are versatile model systems for exploring quantum physics or for the simulation of solid state materials. Meanwhile, they have been created from various atomic species - from alkali metals over alkaline earths to rare earth elements. The latest addition are quantum gases of different kinds of polar molecules. Expectations for quantum gases of heteronuclear molecules are high: Due to their large electric dipole moments, these molecules can interact with each other via long-range interactions - not just via contact interactions as is the case for most atoms. Additionally, they have vibrational and rotational degrees of freedom, with open up new possibilities for quantum simulation. But the same degrees of freedom also pose some challenges. For example, they make the preparation of the quantum gas more difficult, which is typically produced with a combination of laser cooling and evaporative cooling in the atomic case. Molecules mostly lack closed transitions in their spectra, which are required for laser cooling. Therefore, we create our molecular quantum gas from a mixture of two atomic quantum gases. In this work, such an experimental method was developed for fermionic NaK molecules, which is based on the two-photon process Stimulated Raman Adiabatic Passage (STIRAP). Within STIRAP, the hyperfine structure of the chosen intermediate state plays an important role. Experimentally, and with the help of a theoretical model describing the whole process, we find that we produce the most molecules when we use a large one-photon detuning, if the hyperfine structure of the intermediate state is unresolved. In another project, we explored the rotational level structure of the molecular ground state populated by STIRAP. Rotation is closely linked to the electric dipole moment. The superposition of the ground state with the first excited rotational state, for example, has a transition dipole moment of almost 60% of the permanent electric dipole moment. Unfortunately, coherence times of such superpositions are typically short, as the different polarizabilities of the rotational states lead to dephasing in optical traps. However, using a special polarization angle and a small, dc electric field, we can compensate these differences and realize a spin-decoupled magic trap. With this new technique we obtain record coherence times, at least for small molecular densities. For larger densities we observe first indications for dipolar interactions in a bulk gas of polar molecules, which we also model using the moving-average cluster expansion (MACE).
Abstract We spectroscopically investigate a pathway for the conversion of 23Na39K Feshbach molecules into rovibronic ground state molecules via stimulated Raman adiabatic passage. Using photoassociation spectroscopy from the diatomic scattering threshold in the a 3Σ+ potential, we locate the resonantly mixed electronically excited intermediate states ∣ B 1 Π , v = 8 〉 and ∣ c 3 Σ + , v = 30 〉 which, due to their singlet–triplet admixture, serve as an ideal bridge between predominantly a 3Σ+ Feshbach molecules and pure X 1Σ+ ground state molecules. We investigate their hyperfine structure and present a simple model to determine the singlet–triplet coupling of these states. Using Autler–Townes spectroscopy, we locate the rovibronic ground state of the 23Na39K molecule ( ∣ X 1 Σ + , v = 0 , N = 0 〉 ) and the second rotationally excited state N = 2 to unambiguously identify the ground state. We also extract the effective transition dipole moment from the excited to the ground state. Our investigations result in a fully characterized scheme for the creation of ultracold bosonic 23Na39K ground state molecules.
A quantum gas of ultracold polar molecules, with long-range and anisotropic interactions, not only would enable explorations of a large class of many-body physics phenomena but also could be used for quantum information processing. We report on the creation of an ultracold dense gas of potassium-rubidium (40K87Rb) polar molecules. Using a single step of STIRAP (stimulated Raman adiabatic passage) with two-frequency laser irradiation, we coherently transfer extremely weakly bound KRb molecules to the rovibrational ground state of either the triplet or the singlet electronic ground molecular potential. The polar molecular gas has a peak density of 10(12) per cubic centimeter and an expansion-determined translational temperature of 350 nanokelvin. The polar molecules have a permanent electric dipole moment, which we measure with Stark spectroscopy to be 0.052(2) Debye (1 Debye = 3.336 x 10(-30) coulomb-meters) for the triplet rovibrational ground state and 0.566(17) Debye for the singlet rovibrational ground state.
One possibility for the creation of ultracold, high phase space density quantum gases of molecules in the rovibronic ground state relies on first associating weakly-bound molecules from quantum-degenerate atomic gases on a Feshbach resonance and then transferring the molecules via several steps of coherent two-photon stimulated Raman adiabatic passage (STIRAP) into the rovibronic ground state. Here, in ultracold samples of Cs2 Feshbach molecules produced out of ultracold samples of Cs atoms, we observe several optical transitions to deeply-bound rovibrational levels of the excited 0(u)+ molecular potentials with high resolution. At least one of these transitions, although rather weak, allows efficient STIRAP transfer into the deeply-bound vibrational level (see text for symbols)v = 73 > of the singlet X1 sigma(g)+ ground state potential, as recently demonstrated (J. G. Danzl, E. Haller, M. Gustavsson, M. J. Mark, R. Hart, N. Bouloufa, O. Dulieu, H. Ritsch, and H.-C. Nägerl, Science, 2008, 321, 1062). From this level, the rovibrational ground state (see text for symbols)v = 0, J = 0 > can be reached with one more transfer step. In total, our results show that coherent ground state transfer for Cs2 is possible using a maximum of two successive two-photon STIRAP processes or one single four-photon STIRAP process.
We report the creation of ultracold bosonic dipolar ^{23}Na^{39}K molecules in their absolute rovibrational ground state. Starting from weakly bound molecules immersed in an ultracold atomic mixture, we coherently transfer the dimers to the rovibrational ground state using an adiabatic Raman passage. We analyze the two-body decay in a pure molecular sample and in molecule-atom mixtures and find an unexpectedly low two-body decay coefficient for collisions between molecules and ^{39}K atoms in a selected hyperfine state. The preparation of bosonic ^{23}Na^{39}K molecules opens the way for future comparisons between fermionic and bosonic ultracold ground-state molecules of the same chemical species.