This thesis reports on the construction of a novel experimental apparatus to create an ultracold sample of chemical stable $^{23}\rm{Na}^{40}\rm{K}$ polar molecules at their absolute ground states. The long range nature of the dipolar interactions between the ground state molecules, is expected to facilitate to observe new quantum many-body states and to simulate prototypical lattice spin models for exploring quantum magnetism and high $T_c$ superconductivity. The experimental procedures are presented in this thesis including: trapping and cooling $^{23}\rm{Na}$ and $ ^{40}\rm{K}$ atoms to quantum degeneracy, associating weakly bound state molecules with Feshbach resonances, and transferring the Feshbach molecules to the rovibrational ground states via stimulated Raman adiabatic passage. As a result, successful transfer has been demonstrated in our experiment with a single-path transfer efficiency $\simeq 60\%$ via a hyperfine non-resolved intermediate state $\vert d^{3}\Pi, \nu=5, J=1, \Omega=1 \rangle$. In addition, a perturbative theoretical study on the Fermi liquid properties of a single-component weakly-interacting two dimensional dipolar fermions with dipole moments $d$ oriented perpendicularly to the plane of their translational motion is presented in the thesis. When the dipole moments are tilted with respect to the translational plane, the effect of anisotropic interaction appears, and collective excitations in the collisionless regime are studied in this configuration. Furthermore, stable dilute supersolid states with two-dimensional bosonic dipoles are predicted to exist with an additional three-body repulsive contact interaction. These novel quantum effects should be accessible experimentally once the $\rm{Na}\rm{K}$ ground state molecules reach quantum degeneracy by further evaporative cooling.
This thesis reports on the construction of a novel experimental apparatus to create an ultracold sample of chemical stable 23Na40K polar molecules at their absolute ground states. The long range nature of the dipolar interactions between the ground state molecules, is expected to facilitate to observe new quantum many-body states and to simulate prototypical lattice spin models for exploring quantum magnetism and high Tc superconductivity. The experimental procedures are presented in this thesis including: trapping and cooling 23Na and 40K atoms to quantum degeneracy, associating weakly bound state molecules with Feshbach resonances, and transferring the Feshbach molecules to the rovibrational ground states via stimulated Raman adiabatic passage. As a result, successful transfer has been demonstrated in our experiment with a single-path transfer efficiency ≃60% via a hyperfine non-resolved intermediate state ∣d3Π,ν=5,J=1,Ω=1⟩. In addition, a perturbative theoretical study on the Fermi liquid properties of a single-component weakly-interacting two dimensional dipolar fermions with dipole moments d oriented perpendicularly to the plane of their translational motion is presented in the thesis. When the dipole moments are tilted with respect to the translational plane, the effect of anisotropic interaction appears, and collective excitations in the collisionless regime are studied in this configuration. Furthermore, stable dilute supersolid states with two-dimensional bosonic dipoles are predicted to exist with an additional three-body repulsive contact interaction. These novel quantum effects should be accessible experimentally once the NaK ground state molecules reach quantum degeneracy by further evaporative cooling.
We report on the creation of an ultracold dipolar gas of fermionic 23Na40 K molecules in their absolute rovibrational and hyperfine ground state. Starting from weakly bound Feshbach molecules, we demonstrate hyperfine resolved two-photon transfer into the singlet X 1Σ+|v=0,J=0⟩ ground state, coherently bridging a binding energy difference of 0.65 eV via stimulated rapid adiabatic passage. The spin-polarized, nearly quantum degenerate molecular gas displays a lifetime longer than 2.5 s, highlighting NaK's stability against two-body chemical reactions. A homogeneous electric field is applied to induce a dipole moment of up to 0.8 D. With these advances, the exploration of many-body physics with strongly dipolar Fermi gases of 23Na40K molecules is within experimental reach.
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.
We report on the creation of an ultracold dipolar gas of fermionic [superscript 23]Na[superscript 40]Kmolecules in their absolute rovibrational and hyperfine ground state. Starting from weakly bound Feshbach molecules, we demonstrate hyperfine resolved two-photon transfer into the singlet X[superscript 1]Σ[superscript +]|v = 0,J = 0⟩ ground state, coherently bridging a binding energy difference of 0.65 eV via stimulated rapid adiabatic passage. The spin-polarized, nearly quantum degenerate molecular gas displays a lifetime longer than 2.5 s, highlighting NaK’s stability against two-body chemical reactions. A homogeneous electric field is applied to induce a dipole moment of up to 0.8 D. With these advances, the exploration of many-body physics with strongly dipolar Fermi gases of [superscript 23]Na[superscript 40]K molecules is within experimental reach.
The discovery and development of methods to cool, trap and manipulate atomic ensembles have generated a revolution in atomic physics, culminating in the ever expanding research field of ultra-cold matter through the realization of Bose-Einstein condensates (BECs). Since the first realization of BEC more than two decades ago, the majority of studies were concerned with systems displaying short-range contact interaction. Following pioneering experiments in ultra-cold KRb, systems involving ultra-cold mixtures have rose to considerable interest through their capability to form diatomic polar molecules. The long-range character of dipolar particle interactions enables the study of a whole new spectrum of quantum many-body phenomena by giving access to the strongly correlated regime. In this context, NaK is a splendid candidate to investigate dipolar effects due to its large electric dipole moment of $2.72 \, $Debye, its chemical stability and the large history of spectroscopic studies devoted to its ground and excited state manifolds. This thesis reports on the first ever realization of a dual-species degenerate mixture of 23Na and 39K. The experimental apparatus combines two pre-cooled atomic sources into a UHV collection region, where a two-color magneto-optical trap is operated. After transferring both species into an optically plugged quadrupole trap, the 23Na ensemble is cooled by selectively removing the hottest atoms from the trap through microwave transitions, while 39K is sympathetically cooled through its thermal contact to 23Na. Following the transfer into an optical dipole trap, the mixture operation suffers from strong losses as the atomic clouds approach the high-density regime. Interspecies interactions are identified as the system parameter that drives the loss mechanism. In order to realize a quantum degenerate mixture, the dual-species collisional properties are investigated both theoretically and experimentally. By preparing both optically trapped ensembles in the spin state ∣f=1,mf=−1⟩, atom loss spectroscopy is performed in a magnetic field range from 0 to 1000G. The observed features include several s-wave poles and a zero crossing of the interspecies scattering length as well as inelastic two-body contributions in the M=mNa+mK=−2 submanifold. Different magnetic field regions are identified for the purposes of sympathetic cooling of 39K and achieving a quantum degenerate mixture. Forced evaporation creates two Bose-Einstein condensates simultaneously at a magnetic field that provides sizable intra- and interspecies scattering rates needed for fast thermalization. The impact of the differential gravitational sag on the miscibility criterion for the mixture is discussed. The experimental setup and measurements are complemented by theoretical calculations that form a feasibility study of molecular NaK. Starting from ultra-cold Feshbach molecules, the study demonstrates possible pathways for the creation of ultra-cold polar NaK molecules in their absolute electronic and rovibrational ground state. In particular, a multi-channel analysis of the electronic ground and K(4p)+Na(3s) excited state manifold of NaK is presented. It analyzes the spin character of both the Feshbach molecular state and the electronically excited intermediate states and discusses possible coherent two-photon transfer paths from Feshbach molecules to rovibronic ground state molecules. %The theoretical study is complemented by the demonstration of STIRAP transfer from the X1Σ+(v=0) state to the a3Σ+ manifold on a molecular beam experiment. The experimental results serve as a promising starting point for the magnetoassociation into quantum degenerate 23Na39K Feshbach molecules. The theoretical analysis assures qualitative understanding as well as quantitative statements for the feasibility of the subsequent ground state conversion. In combination, they fill a critical gap towards the creation of chemically stable ultra-cold molecular Bose-Einstein condensates of NaK.
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 assembly and coherent control of ultracold molecules have opened new horizons in quantum science with applications in ultracold chemistry, quantum information, quantum simulation, precision metrology and fundamental physics. While considerable progress has been achieved in controlling diatomic molecules at ultracold temperatures, extending to atom-diatom collisions and triatomic systems introduces additional internal structure, anisotropy, and interaction complexity, enabling access to many-body phenomena. This dissertation presents a detailed theoretical study on the production and stabilization of ultracold alkali-metal triatomic molecules, with a particular focus on the NaK2 molecular species. First, long-range photoassociation in ultracold NaK(X^1Σ+) + K(4s) mixtures is investigated near the molecular transition X^1Σ+ → b^3Π. Photoassociation rates into weakly bound trimers in the electronically excited 3^2A' state are evaluated under experimentally relevant conditions. The calculated photoassociation rates indicate experimentally feasible and spectrally selective routes for detecting ultracold atom–diatom photoassociation resonances, while suppressing competing diatomic loss channels. Second, a microwave-assisted association mechanism is introduced for coherently binding ultracold atoms and polar molecules into weakly bound triatomic molecules on the ground-state 1^2A' potential energy surface. This process relies on the interaction between the electric component of the microwave field and the permanent electric dipole moment of the NaK molecule. In the presence of the anisotropic atom–diatom potential, which couples the molecular rotation to the relative angular motion, the microwave field can drive transitions from scattering states to weakly bound trimer states entirely in the electronic ground-state of the triatomic molecule, without involving spontaneous emission. This process is therefore intrinsically coherent and particularly suited to closed-shell polar molecules for which magnetically tunable Feshbach resonances are weak or absent. Finally, candidate pathways toward coherent population transfer to the absolute rovibronic ground state of NaK2 are explored using bridge states belonging to the excited 3^2A' electronic state, such as those identified in [Ref.1]. The relevant potential energy surfaces, transition dipole moments, and rovibrational structures are analyzed, revealing favorable conditions for future stimulated Raman adiabatic passage scheme. The theoretical modeling combines high-level electronic-structure calculations with nuclear-motion methods across multiple energy and length scales. Three-dimensional potential energy surfaces and electronic transition dipole moment surfaces were obtained from ab initio multireference configuration interaction calculations employing effective-core pseudopotentials and core-polarization potentials. Nuclear motion was treated using coupled-channel methods for describing weakly bound states and discrete variable representation methods for deeply bound rovibrational states. The resulting wavefunctions were subsequently used to evaluate Franck–Condon factors, photo- and microwave association rates, and transition strengths relevant to experimental implementation. Overall, this dissertation provides an extensive theoretical framework for the formation, detection and ground-state stabilization of ultracold NaK2 trimers. Reference: [1] J. Cao, B.-Y. Wang, H. Yang, Z.-J. Fan, Z. Su, J. Rui, B. Zhao, and J.-W. Pan, “Observation of photoassociation resonances in ultracold atom-molecule collisions,” Phys. Rev. Lett., vol. 132, p. 093403, 2024.