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Dipolar evaporation of reactive molecules to below the Fermi temperature

Giacomo Valtolina, Kyle Matsuda, William G. Tobias, Jun-Ru Li, Luigi De Marco, Jun Ye

Published Jan 1, 2020• 93 citations
OpenAlex

Abstract

Abstract The control of molecules is key to the investigation of quantum phases, in which rich degrees of freedom can be used to encode information and strong interactions can be precisely tuned1. Inelastic losses in molecular collisions2–5, however, have greatly hampered the engineering of low-entropy molecular systems6. So far, the only quantum degenerate gas of molecules has been created via association of two highly degenerate atomic gases7, 8. Here we use an external electric field along with optical lattice confinement to create a two-dimensional Fermi gas of spin-polarized potassium–rubidium (KRb) polar molecules, in which elastic, tunable dipolar interactions dominate over all inelastic processes. Direct thermalization among the molecules in the trap leads to efficient dipolar evaporative cooling, yielding a rapid increase in phase-space density. At the onset of quantum degeneracy, we observe the effects of Fermi statistics on the thermodynamics of the molecular gas. These results demonstrate a general strategy for achieving quantum degeneracy in dipolar molecular gases in which strong, long-range and anisotropic dipolar interactions can drive the emergence of exotic many-body phases, such as interlayer pairing and p-wave superfluidity.

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Ultracold polar molecular quantum gases promise to open new research directions ranging from the study of ultra-cold chemistry, precision measurements to novel quantum phase transitions. Based on the preparation of high-phase space density gases of polar KRb molecules [1–3], I will discuss the control of dipolar collisions and chemical reactions of polar molecules in a regime where quantum statistics, single scattering partial waves, and quantum threshold laws play a dominant role [4]. In particular, I will point out the crucial role of electric dipole-dipole interactions [5] and external confinement [6] in determining the chemical reaction rate. Finally, I will discuss prospects of reaching quantum degeneracy in bialkali samples of polar molecules and prospects for these systems as novel dipolar quantum many-body systems.

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Ultracold polar molecules possess long-range, anisotropic, and tunable dipolar interactions, providing unique opportunities to probe novel quantum phenomena. However, experimental progress has been hindered by excessive two-body loss, which also limits further cooling via evaporation. Recent work shows the loss can be mitigated by confining molecules in a two-dimensional geometry. However, a general approach for tuning molecular interactions in a full three-dimensional (3D) stable system has been lacking. Here, we demonstrate the use of an electric field-induced shielding resonance to suppress the reactive loss by a factor of 30 while preserving elastic, long-range dipolar interactions in a bulk gas of ultracold 40K87Rb molecules in 3D. The favorable ratio of elastic to inelastic collisions enables direct thermalization, the rate of which depends on the angle between the collisional axis and the dipole orientation controlled by an external electric field. This is a direct manifestation of the anisotropic dipolar interaction. We further achieve dipolar-interaction-mediated evaporative cooling in 3D. This work demonstrates control of a long-lived bulk quantum gas system with tunable long-range interactions, paving the way for the study of collective quantum many-body physics.

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Ultracold Polar KRb Molecules in Optical Lattices

Brian Neyenhuis

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.

•Jan 1, 2012•3 citations
Abstract The control of molecules is key to the investigation of quantum phases, in which rich degrees of freedom can be used to encode information and strong interactions can be precisely tuned1. Inelastic losses in molecular collisions2–5, however, have greatly hampered the engineering of low-entropy molecular systems6. So far, the only quantum degenerate gas of molecules has been created via association of two highly degenerate atomic gases7, 8. Here we use an external electric field along with optical lattice confinement to create a two-dimensional Fermi gas of spin-polarized potassium–rubidium (KRb) polar molecules, in which elastic, tunable dipolar interactions dominate over all inelastic processes. Direct thermalization among the molecules in the trap leads to efficient dipolar evaporative cooling, yielding a rapid increase in phase-space density. At the onset of quantum degeneracy, we observe the effects of Fermi statistics on the thermodynamics of the molecular gas. These results demonstrate a general strategy for achieving quantum degeneracy in dipolar molecular gases in which strong, long-range and anisotropic dipolar interactions can drive the emergence of exotic many-body phases, such as interlayer pairing and p-wave superfluidity.
Abstract Ultracold polar molecules offer strong electric dipole moments and rich internal structure, which makes them ideal building blocks to explore exotic quantum matter 1–9 , implement quantum information schemes 10–12 and test the fundamental symmetries of nature 13 . Realizing their full potential requires cooling interacting molecular gases deeply into the quantum-degenerate regime. However, the intrinsically unstable collisions between molecules at short range have so far prevented direct cooling through elastic collisions to quantum degeneracy in three dimensions. Here we demonstrate evaporative cooling of a three-dimensional gas of fermionic sodium–potassium molecules to well below the Fermi temperature using microwave shielding. The molecules are protected from reaching short range with a repulsive barrier engineered by coupling rotational states with a blue-detuned circularly polarized microwave. The microwave dressing induces strong tunable dipolar interactions between the molecules, leading to high elastic collision rates that can exceed the inelastic ones by at least a factor of 460. This large elastic-to-inelastic collision ratio allows us to cool the molecular gas to 21 nanokelvin, corresponding to 0.36 times the Fermi temperature. Such cold and dense samples of polar molecules open the path to the exploration of many-body phenomena with strong dipolar interactions.
Quantum gases of polar molecules have recently emerged as a powerful platform for exploring exotic many-body dynamics and correlated quantum behavior. To achieve the full potential of this platform, the production of deeply degenerate quantum gases of molecules in arbitrary confinement geometries is necessary. Here, we successfully evaporate fermionic KRb molecules in both 3D and quasi-2D geometries to well below their Fermi temperatures utilizing dipolar collisions. As we evaporate deeper into degeneracy in both geometries, we enter the Pauli-blocked regime with polar molecules, which we independently confirm for the first time by measuring the Pauli suppression of elastic collisions. Moreover, the Pauli suppression of collisions contributes to the limitation of our final molecular temperature to about 25% of the Fermi temperature in both geometries, particularly limiting quasi-2D evaporation where the Pauli blockade drastically reduces an otherwise large elastic to inelastic scattering ratio. This work demonstrates the production of degenerate Fermi gases of polar molecules both in a 3D harmonic trap and in mono- and bi-layer 2D configurations. Further, our work explores the fundamental limits on evaporation of molecular Fermi gases set by the Pauli-exclusion principle, which could be overcome in the future by introducing distinguishable scattering partners.
Fermi statistics suppress the elastic collisions that rethermalize a Fermi gas during evaporative cooling, creating a fundamental low-temperature bottleneck for producing quantum degenerate gases. We show that, for shielded single-component ultracold dipolar molecular Fermi gases in the Wigner threshold regime, this bottleneck is governed by universal threshold laws fixed by the effective dimensionality of the gas. In this regime, Fermi suppression of rethermalization scales quadratically with temperature in 3D but only linearly in 2D. Consequently, the thermalization-to-loss ratio is more favorable in 2D than in 3D, and these results suggest that 2D geometries are better suited for reaching deep degeneracy. We also present ab initio close-coupling calculations that agree well with experimental measurements on Fermi degenerate gases of KRb molecules, supporting our conclusions.
Ultracold polar molecular quantum gases promise to open new research directions ranging from the study of ultra-cold chemistry, precision measurements to novel quantum phase transitions. Based on the preparation of high-phase space density gases of polar KRb molecules [1–3], I will discuss the control of dipolar collisions and chemical reactions of polar molecules in a regime where quantum statistics, single scattering partial waves, and quantum threshold laws play a dominant role [4]. In particular, I will point out the crucial role of electric dipole-dipole interactions [5] and external confinement [6] in determining the chemical reaction rate. Finally, I will discuss prospects of reaching quantum degeneracy in bialkali samples of polar molecules and prospects for these systems as novel dipolar quantum many-body systems.
Ultracold polar molecules possess long-range, anisotropic, and tunable dipolar interactions, providing unique opportunities to probe novel quantum phenomena. However, experimental progress has been hindered by excessive two-body loss, which also limits further cooling via evaporation. Recent work shows the loss can be mitigated by confining molecules in a two-dimensional geometry. However, a general approach for tuning molecular interactions in a full three-dimensional (3D) stable system has been lacking. Here, we demonstrate the use of an electric field-induced shielding resonance to suppress the reactive loss by a factor of 30 while preserving elastic, long-range dipolar interactions in a bulk gas of ultracold 40K87Rb molecules in 3D. The favorable ratio of elastic to inelastic collisions enables direct thermalization, the rate of which depends on the angle between the collisional axis and the dipole orientation controlled by an external electric field. This is a direct manifestation of the anisotropic dipolar interaction. We further achieve dipolar-interaction-mediated evaporative cooling in 3D. This work demonstrates control of a long-lived bulk quantum gas system with tunable long-range interactions, paving the way for the study of collective quantum many-body physics.
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.