We examine the potential-energy curves and polarization of the dipole moments of two static polar molecules under the influence of an external dc electric field and their anisotropic dipole-dipole interaction. We model the molecules as quantum rigid rotors to take their rotational degrees of freedom into account and consider a selection of linear, symmetric, and asymmetric top molecules. We provide a comprehensive examination of the energy curves and polarization of the dipoles for varying intermolecular separation and direction of the electric field and find that the properties of the molecules depend strongly on the field's direction at short separations, showing the importance of accounting for molecular rotation. The latter provides insight into the possible effects of accounting for rotational degrees of freedom in molecular dipolar gases. Published by the American Physical Society 2024
We examine the potential-energy curves and polarization of the dipole moments of two static polar molecules under the influence of an external dc electric field and their anisotropic dipole-dipole interaction. We model the molecules as quantum rigid rotors to take their rotational degrees of freedom into account and consider a selection of linear, symmetric, and asymmetric top molecules. We provide a comprehensive examination of the energy curves and polarization of the dipoles for varying intermolecular separation and direction of the electric field and find that the properties of the molecules depend strongly on the field's direction at short separations, showing the importance of accounting for molecular rotation. The latter provides insight into the possible effects of accounting for rotational degrees of freedom in molecular dipolar gases. Published by the American Physical Society 2024
Inelastic collisions between dipolar molecules, assumed to be trapped in a static electric field at cold (> 10−3K) temperatures, are investigated and compared with elastic collisions. For molecules with a Λ-doublet energy-level structure, a dipole moment arises because of the existence of two nearly degenerate states of opposite parity, and the collision of two such dipoles can be solved entirely analytically in the energy range of interest. Cross sections and rate constants are found to satisfy simple, universal formulas. In contrast, for molecules in a Σ electronic ground state, the static electric field induces a dipole moment in one of three rotational sublevels. Collisions between two rotor dipoles are calculated numerically; the results scale simply with molecule mass, rotational constant, dipole moment, and field strength. It might be expected that any particles interacting only under the influence of the dipole-dipole interaction would show similar behavior; however, the most important and general result of this research is that at cold temperatures inelastic rate constants and cross sections for dipoles depend strongly upon the internal structure of the molecules. The most prominent difference between the Λ-doublet and rotor molecules is variation of the inelastic cross section with applied field strength. For Λ-doublet dipoles, cross sections decrease with increasing field strength. For rotor dipoles, cross sections increase proportionally with the square of field strength. Furthermore, the rate constants of the two types of molecules depend very differently on the angular orientations of the dipoles in the electric field.
We establish a correspondence between the electric dipole matrix elements of a polyatomic symmetric top molecule in a state with nonzero projection of the total angular momentum on the symmetry axis of the molecule and the magnetic dipole matrix elements of a magnetic dipole associated with an elemental spin F. It is shown that this correspondence makes it possible to perform quantum simulation of the single-particle spectrum and the dipole-dipole interactions of magnetic dipoles in a static external magnetic field B with symmetric top molecules subject to a static external electric field EDC. We further show that no such correspondence exists for 1Σ molecules in static fields, such as the alkali metal dimers. The effective spin angular momentum of the simulated magnetic dipole corresponds to the rotational angular momentum of the symmetric top molecule, and so quantum simulation of arbitrarily large integer spins is possible. Further, taking the molecule CH3F as an example, we show that the characteristic dipole-dipole interaction energies of the simulated magnetic dipole are a factor of 620, 600, and 310 larger than for the highly magnetic atoms Chromium, Erbium, and Dysprosium, respectively. We present several applications of our correspondence for many-body physics, including long-range and anisotropic spin models with arbitrary integer spin S using symmetric top molecules in optical lattices, quantum simulation of molecular magnets, and spontaneous demagnetization of Bose-Einstein condensates due to dipole-dipole interactions. Our results are expected to be relevant as cold symmetric top molecules reach quantum degeneracy through Stark deceleration and opto-electrical cooling.
This thesis contains a study of ultracold paramagnetic atoms or polar molecules characterized by a long-range anisotropic dipolar interaction. We particularly focus on two aspects of ultracold dipolar gases. In the first problem the ground state properties of dipolar Bose-Einstein condensates (BEC) are investigated. This problem has gained importance due to recent experimental advances in achieving a condensate of Chromium atoms and ongoing research to produce quantum degenerate polar molecules. In the second problem, we consider possible applications of ultracold polar molecules to rotation sensing and interferometry. First, we concentrate on the interplay between the trapping geometry and dipole-dipole interaction for a polarized dipolar bosonic condensate. As the dipole-dipole interaction is attractive along the polarized direction, the lowest energy state of the BEC is always a collapsed state. However by applying a trapping potential along the polarization direction it is possible to achieve a metastable dipolar BEC. By numerically solving the Gross-Pitaevskii equation, we show that below a critical interaction strength, a metastable state exists depending on the trapping geometry. We also show that a novel feature of dipolar BEC is the appearance of different structural metastable ground states for certain combinations of trapping geometry and particle number. Next, by mixing in single component fermions we show that dipolar BEC can be stabilized against collapse in pancake shaped or cylindrical traps. We also show that the excitation spectrum of the BEC may have a minimum for non-zero momentum, termed a “roton minimum”. This minimum leads to a transition to stable or metastable density-wave states depending on the density of the bosons and boson-fermion interaction strength. In the second problem, we study a proposal for a large-angle coherent beam splitter for polar molecules. By taking into account the effect of a quasi-static external electric field on the rotational levels of the polarized molecules we show that it is possible to coherently split a stationary cloud of molecules into two counter-propagating components. We then investigate the effect of longitudinal acceleration on the transverse motion of the particles, assuming that the longitudinal motion of the molecules can be approximated classically by a wave packet with some mean velocity while the transverse motion is governed by quantum mechanics. We propose a particular time-dependent shape of acceleration to minimize the excitations in the transverse motion. Our theory is also applicable to the general case of particles moving along a circular guide with time-dependent longitudinal velocity. In addition, we include the effects of velocity fluctuations due to noise in the accelerating field.
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).
Two elementary models of molecular structure are used to investigate inelastic collisions in cold trapped dipolar gases. A two-state model of a polar molecule (such as one with a Λ-doublet) permits analytic description of the inelastic collision process at energies considerably higher than the gap energy, predicting rate constants and cross sections given by elementary formulae. Alternatively, a three-state model of a rotor molecule in an electric field is investigated, with resultant rate constants and cross sections scaling simply with molecular mass, rotational constant, dipole moment and polarizing field strength. Semiclassical inelastic collision cross sections and rate constants are demonstrated to depend strongly on the model used, especially as regards their dependence on the polarizing field. Inelastic cross sections among doublet dipoles decrease with increasing field strength, while they increase in proportion to the square of the field strength for collisions between rotor dipoles.