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arXiv:1504.04578 · Physical Review Letters

Ultracold Dipolar Molecules Composed of Strongly Magnetic Atoms

Albert Frisch, Manfred J. Mark, K. Aikawa, Simon Baier, Rudolf Grimm, Alexander N. Petrov, Svetlana Kotochigova, Goulven Quéméner, Maxence Lepers, Olivier Dulieu, Francesca Ferlaino

Published Nov 9, 2015• 95 citations
arXivHTMLPDF

Abstract

In a combined experimental and theoretical effort, we demonstrate a novel type of dipolar system made of ultracold bosonic dipolar molecules with large magnetic dipole moments. Our dipolar molecules are formed in weakly bound Feshbach molecular states from a sample of strongly magnetic bosonic erbium atoms. We show that the ultracold magnetic molecules can carry very large dipole moments and we demonstrate how to create and characterize them, and how to change their orientation. Finally, we confirm that the relaxation rates of molecules in a quasi-two-dimensional geometry can be reduced by using the anisotropy of the dipole-dipole interaction and that this reduction follows a universal dipolar behavior.

DOI
10.1103/physrevlett.115.203201

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In a combined experimental and theoretical effort, we demonstrate a novel type of dipolar system made of ultracold bosonic dipolar molecules with large magnetic dipole moments. Our dipolar molecules are formed in weakly bound Feshbach molecular states from a sample of strongly magnetic bosonic erbium atoms. We show that the ultracold magnetic molecules can carry very large dipole moments and we demonstrate how to create and characterize them, and how to change their orientation. Finally, we confirm that the relaxation rates of molecules in a quasi-two-dimensional geometry can be reduced by using the anisotropy of the dipole-dipole interaction and that this reduction follows a universal dipolar behavior.
Creation of a strongly dipolar gas of ultracold ground-state 23Na87Rb^{23}\rm{Na}^{87}\rm{Rb}23Na87Rb molecules
We report the successful production of an ultracold sample of absolute ground-state 23Na87Rb^{23}\rm{Na}^{87}\rm{Rb}23Na87Rb molecules with a large induced electric dipole moment. Starting from weakly-bound Feshbach molecules formed via magneto-association, the lowest rovibrational and hyperfine level of the electronic ground state is populated following a high efficiency and high resolution two-photon Raman process. The high purity absolute ground-state samples have up to 8000 molecules and densities of over 101110^{11}1011 cm−3^{-3}−3. With an external electric field, we have induced an effective dipole moment over one Debye, enough to provide truly strong and long-range dipolar interactions. Bimolecular reaction between ground-state 23Na87Rb^{23}\rm{Na}^{87}\rm{Rb}23Na87Rb molecules is endothermic, but we still observed a rather fast decay of the molecular sample. Our results pave the way toward investigation of ultracold molecular collisions in a fully controlled manner, and possibly to quantum gases of ultracold bosonic molecules with strong dipolar interactions.
Abstract This paper reviews recent advances in the study of strongly interacting systems of dipolar molecules. Heteronuclear molecules feature large and tunable electric dipole moments, which give rise to long-range and anisotropic dipole–dipole interactions. Ultracold samples of dipolar molecules with long-range interactions offer a unique platform for quantum simulations and the study of correlated many-body physics. We provide an introduction to the physics of dipolar quantum gases, both electric and magnetic, and summarize the multipronged efforts to bring dipolar molecules into the quantum regime. We discuss in detail the recent experimental progress in realizing and studying strongly interacting systems of polar molecules trapped in optical lattices, with particular emphasis on the study of interacting spin systems and non-equilibrium quantum magnetism. Finally, we conclude with a brief discussion of the future prospects for studies of strongly interacting dipolar molecules.
Strongly interacting ultracold dipolar molecules are a rich platform for quantum information and quantum simulation of phenomena relevant to condensed matter systems. This dissertation presents novel theoretical and computational studies of ultracold dipolar molecules relevant to these areas in three broad categories.First, the path integral ground state quantum Monte Carlo method is extended to simulations with both translational and rotational degrees of freedom, including the development of a novel estimator of the elementary excitation energies of a system with these degrees of freedom based on the well known Feynman-Bijl approximation. This is then used to study dipolar molecular ensembles confined to one-dimensional optical lattices. The ground state phase diagram is characterized with both a mean-field method and the aforementioned quantum Monte Carlo method. A quantum phase transition is found for very short optical lattice spacings or very large dipole moments. The prospects for experimentally realizing a system which exhibits this phase transition are discussed.Second, the path integral ground state quantum Monte Carlo method is utilized to study the ground state of dipole molecules confined to two-dimensional optical lattices. On square lattices a crossover from a weakly interacting disordered phase to a strongly interacting striped phase is found for short lattice spacings or large dipole moments. On triangular lattices a crossover between a disordered phase and a completely polarized phase is found, also for short lattice spacings or large dipole moments. The relevance of such simulations to self-assembled dipolar crystals in two dimensions is discussed and simulation results of these systems are presented. Simulations of polarized and harmonically confined molecular systems in two dimensions with translations and rotations are also presented and a realistic interaction potential using highly accurate ab initio quantum chemistry techniques is calculated for LiH--LiH interactions as a preliminary step toward developing a high quality trial wave function for the simulation of systems possessing both translational and rotational degrees of freedom.Finally, several novel applications for dipolar molecules confined to optical lattices are proposed. An experimental realization of a topological phase using 2Sigma^2\\Sigma2Sigma ground state molecules with applied near resonant microwave fields and transverse magnetic fields is proposed. A method to create an array of dipole-coupled two-level molecules exhibiting superradiance and possessing novel spectroscopic properties using 1Sigma^1\\Sigma1Sigma ground state molecules in the combination of a far off-resonant laser field and a moderate magnetic field is proposed. Additionally, a method to create entangled pairs of molecules using closed-shell dipolar molecules immersed in an intense far off-resonant laser field is reviewed and an extension in which parallel optical lattices are merged and molecules are allowed to collide in the presence of a far off-resonant laser field is proposed. Simulation results are presented indicating that a significant amount of entanglement may be generated in such a way in realistic molecular systems.
We report the successful production of an ultracold sample of absolute ground-state ^{23}Na^{87}Rb molecules. Starting from weakly bound Feshbach molecules formed via magnetoassociation, the lowest rovibrational and hyperfine level of the electronic ground state is populated following a high-efficiency and high-resolution two-photon Raman process. The high-purity absolute ground-state samples have up to 8000 molecules and densities of over 10^{11} cm^{-3}. By measuring the Stark shifts induced by external electric fields, we determined the permanent electric dipole moment of the absolute ground-state ^{23}Na^{87}Rb and demonstrated the capability of inducing an effective dipole moment over 1 D. Bimolecular reaction between ground-state ^{23}Na^{87}Rb molecules is endothermic, but we still observed a rather fast decay of the molecular sample. Our results pave the way toward investigation of ultracold molecular collisions in a fully controlled manner and possibly to quantum gases of ultracold bosonic molecules with strong dipolar interactions.
Dipolar quantum gases, encompassing atoms and molecules with significant dipole moments, exhibit unique long-range and anisotropic dipole-dipole interactions (DDI), distinguishing them from systems dominated by short-range contact interactions. This review explores their behavior across dimensions, focusing on magnetic atoms in quasi-2D in comparison to 3D. In 3D, strong DDI leads to phenomena like anisotropic superfluidity, quantum droplets stabilized by Lee-Huang-Yang corrections, and supersolid states with density modulations. In 2D, we discuss a new scenario where DDI induces angle-dependent Berezinskii-Kosterlitz-Thouless transitions and potential supersolidity, as suggested by recent experimental realizations of strongly dipolar systems in quasi-2D geometries. We identify key challenges for future experimental and theoretical work on strongly dipolar 2D systems. The review concludes by highlighting how these unique 2D dipolar systems could advance fundamental research as well as simulate novel physical phenomena.
We report on the creation of bosonic NaCs molecules in their absolute rovibrational ground state via stimulated Raman adiabatic passage. We create ultracold gases with up to 22 000 dipolar NaCs molecules at a temperature of 300(50) nK and a peak density of 1.0(4)×10^{12} cm^{-3}. We demonstrate comprehensive quantum state control by preparing the molecules in a specific electronic, vibrational, rotational, and hyperfine state. We measure the ground state ac polarizability at 1064 nm along with the two-body loss rate, which we find to be universal. Employing the tunability and strength of the permanent electric dipole moment of NaCs, we induce dipole moments of up to 2.6 D at a dc electric field of 2.1(2) kV/cm and demonstrate strong microwave coupling between the two lowest rotational states with a Rabi frequency of 2π×45 MHz. A large electric dipole moment, accessible at relatively small electric fields, makes ultracold gases of NaCs molecules well suited for the exploration of strongly interacting phases of dipolar quantum matter.