Polar quantum gases represent promising platforms for studying many-body physics and strongly correlated systems with possible applications e.g. in quantum simulation or quantum computation. Due to their large permanent electric dipole moment polar molecules in electric field exhibit strong long-range anisotropic dipole-dipole interactions (DDIs). The creation and trapping of ultracold dipolar diatomic molecules of various species are feasible in many experimental groups nowadays. However long time trapping is still a challenge even in the case of the so called nonreactive molecules which are supposed to be immune against inelastic collisions in their absolute ground state [1] . Various hypothesis have been invoked to explain the possible mechanisms behind the trapping loss, however the check of their pertinence is not trivial since the final products can not be easily detected [2] . To overcome the loss processes we propose the suppression of inelastic collisions between molecules using optical shielding (OS). OS relies on the modification of long-range interactions between ground-state and excited molecules by laser light. The first experimental proof of OS process was demonstrated in case of the collision between identical ultracold alkali-metal atoms [3] .
Polar quantum gases represent promising platforms for studying many-body physics and strongly correlated systems with possible applications e.g. in quantum simulation or quantum computation. Due to their large permanent electric dipole moment polar molecules in electric field exhibit strong long-range anisotropic dipole-dipole interactions (DDIs). The creation and trapping of ultracold dipolar diatomic molecules of various species are feasible in many experimental groups nowadays. However long time trapping is still a challenge even in the case of the so called nonreactive molecules which are supposed to be immune against inelastic collisions in their absolute ground state [1] . Various hypothesis have been invoked to explain the possible mechanisms behind the trapping loss, however the check of their pertinence is not trivial since the final products can not be easily detected [2] . To overcome the loss processes we propose the suppression of inelastic collisions between molecules using optical shielding (OS). OS relies on the modification of long-range interactions between ground-state and excited molecules by laser light. The first experimental proof of OS process was demonstrated in case of the collision between identical ultracold alkali-metal atoms [3] .
We propose a method to suppress the chemical reactions between ultracold bosonic ground-state ^{23}Na^{87}Rb molecules based on optical shielding. By applying a laser with a frequency blue-detuned from the transition between the lowest rovibrational level of the electronic ground state X^{1}Σ^{+}(v_{X}=0,j_{X}=0), and the long-lived excited level b^{3}Π_{0}(v_{b}=0,j_{b}=1), the long-range dipole-dipole interaction between the colliding molecules can be engineered, leading to a dramatic suppression of reactive and photoinduced inelastic collisions, for both linear and circular laser polarizations. We demonstrate that the spontaneous emission from b^{3}Π_{0}(v_{b}=0,j_{b}=1) does not deteriorate the shielding process. This opens the possibility for a strong increase of the lifetime of cold molecule traps and for an efficient evaporative cooling. We also anticipate that the proposed mechanism is valid for alkali-metal diatomics with sufficiently large dipole-dipole interactions.
Abstract Ultracold temperatures in dilute quantum gases opened the way to an exquisite control of matter at the quantum level. Here we focus on the control of ultracold atomic collisions using a laser to engineer their interactions at large interatomic distances. We show that the entrance channel of two colliding ultracold atoms can be coupled to a repulsive collisional channel by the laser light so that the overall interaction between the two atoms becomes repulsive: this prevents them to come close together and to undergo inelastic processes, thus protecting the atomic gases from unwanted losses. We illustrate such an optical shielding (OS) mechanism with 39 K and 133 Cs atoms colliding at ultracold temperature (<1 μK). The process is described in the framework of the dressed-state picture and we then solve the resulting stationary coupled Schrödinger equations. The role of spontaneous emission and photoinduced inelastic scattering is also investigated as possible limitations of the shielding efficiency. We predict an almost complete suppression of inelastic collisions over a broad range of Rabi frequencies and detunings from the 39 K D2 line of the OS laser, both within the [0, 200 MHz] interval. We found that the polarization of the shielding laser has a minor influence on this efficiency. This proposal could easily be formulated for other bialkali-metal pairs as their long-range interaction are all very similar to each other.
The creation of a gas of ultracold polar molecules with a high phase space density brings new possibilities beyond experiments with ultracold atomic gases. In particular, long-range, anisotropic, and tunable dipole-dipole interactions open the way for novel quantum gases, with applications including strongly correlated many-body systems, and ultracold chemistry. This thesis will present the final steps to complete control over both internal and external degrees of freedom of the molecule which allows us to control, and even completely suppress, the chemical reactions between molecules. First, the control over internal states has been achieved through coherent state transfer to the ro-vibronic ground state and coherent manipulations of the hyperfine and rotational states with microwave radiation. Second, external degrees of freedom are controlled by loading the gas into an optical lattice. With the molecules loaded into a one-dimensional lattice, the orientation of the molecular collisions is controlled by manipulating both internal (hyperfine states) and external (motional states in the direction of tight confinement) degrees of freedom. Most striking is that by preparing the molecules all in the lowest band of the lattice in the same internal state, the molecular collisions can only occur in a side-by-side" orientation, where the chemical reaction rate is suppressed by the repulsive dipole-dipole interactions. The chemical reaction can be suppressed completely by further constraining the motion in the trap in a strong 3D lattice. Here we see lifetimes longer than 20 s, limited by o-resonant light scattering. Finally, the ac polarizability of the molecules is explored and controlled. The different rotational states of the molecule have different polarizabilities and will experience a different trapping force in both the optical dipole trap or lattice. We show that there is a magic angle" between the quantization axis and the polarization of the trapping laser at which the polarizabilities of two different rotational states can be matched, eliminating dephasing and allowing for coherent manipulations between rotational states.
We study polar alkali-metal dimer scattering in a quasi-one-dimensional geometry for both reactive and nonreactive species. Elastic and reactive rates are computed as a function of the amplitude of a static electric field within a purely long-range model with suitable boundary conditions at shorter range. We describe the diatomic molecules as rigid rotors and results are compared to the fixed-dipole approximation. We show in particular that for molecules with a sufficiently strong induced dipole moment oriented perpendicular to the trap axis, the long-range repulsive interaction leads to the suppression of short-range processes. Such shielding effect occurs for both reactive and nonreactive molecules, preventing two-body reactions as well as losses due to complex-mediated processes [M. Mayle et al., Phys. Rev. A 85, 062712 (2012)] from occurring. The present results demonstrate the possibility to suppress loss rates in current ultracold molecule experiments using one-dimensional confinement.
The prospects for shielding ultracold, paramagnetic, dipolar molecules from inelastic and chemical collisions are investigated. Molecules placed in their first rotationally excited states are found to exhibit effective long-range repulsion for applied electric fields above a certain critical value, as previously shown for nonparamagnetic molecules. This repulsion can safely allow the molecules to scatter while reducing the risk of inelastic or chemically reactive collisions. Several molecular species of $^{2}\mathrm{\ensuremath{\Sigma}}$ molecules of experimental interest---RbSr, SrF, BaF, and YO---are considered, and all are shown to exhibit orders of magnitude suppression in quenching rates in a sufficiently strong laboratory electric field. It is further shown that, for these molecules described by Hund's coupling case (b), electronic and nuclear spins play the role of spectator with respect to the shielding.
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).