Tunable itinerant spin dynamics with polar molecules.

Strongly interacting spins underlie many intriguing phenomena and applications1-4 ranging from magnetism to quantum information processing. Interacting spins combined with motion show exotic spin transport phenomena, such as superfluidity arising from pairing of spins induced by spin attraction5,6. To understand these complex phenomena, an interacting spin system with high controllability is desired. Quantum spin dynamics have been studied on different platforms with varying capabilities7-13. Here we demonstrate tunable itinerant spin dynamics enabled by dipolar interactions using a gas of potassium-rubidium molecules confined to two-dimensional planes, where a spin-1/2 system is encoded into the molecular rotational levels. The dipolar interaction gives rise to a shift of the rotational transition frequency and a collision-limited Ramsey contrast decay that emerges from the coupled spin and motion. Both the Ising and spin-exchange interactions are precisely tuned by varying the strength and orientation of an electric field, as well as the internal molecular state. This full tunability enables both static and dynamical control of the spin Hamiltonian, allowing reversal of the coherent spin dynamics. Our work establishes an interacting spin platform that allows for exploration of many-body spin dynamics and spin-motion physics using the strong, tunable dipolar interaction.

Dipolar evaporation of reactive molecules to below the Fermi temperature.

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.

Dynamical Generation of Spin Squeezing in Ultracold Dipolar Molecules.

We study a bulk fermionic dipolar molecular gas in the quantum degenerate regime confined in a two-dimensional geometry. Using two rotational states of the molecules, we encode a spin 1/2 degree of freedom. To describe the many-body spin dynamics of the molecules, we derive a long-range interacting XXZ model valid in the regime where motional degrees of freedom are frozen. Because of the spatially extended nature of the harmonic oscillator modes, the interactions in the spin model are very long ranged, and the system behaves close to the collective limit, resulting in robust dynamics and generation of entanglement in the form of spin squeezing even at finite temperature and in the presence of dephasing and chemical reactions. We discuss how the internal state structure can be exploited to realize time reversal and enhanced metrological sensing protocols.

Thermalization and Sub-Poissonian Density Fluctuations in a Degenerate Molecular Fermi Gas.

We observe thermalization in the production of a degenerate Fermi gas of polar ^{40}K^{87}Rb molecules. By measuring the atom-dimer elastic scattering cross section near the Feshbach resonance, we show that Feshbach molecules rapidly reach thermal equilibrium with both parent atomic species. Equilibrium is essentially maintained through coherent transfer to the ground state. Sub-Poissonian density fluctuations in Feshbach and ground-state molecules are measured, giving an independent characterization of degeneracy and directly probing the molecular Fermi-Dirac distribution.

Sisyphus Laser Cooling of a Polyatomic Molecule.

We perform magnetically assisted Sisyphus laser cooling of the triatomic free radical strontium monohydroxide (SrOH). This is achieved with principal optical cycling in the rotationally closed P(N^{''}=1) branch of either the X[over ˜]^{2}Σ^{+}(000)↔A[over ˜]^{2}Π_{1/2}(000) or the X[over ˜]^{2}Σ^{+}(000)↔B[over ˜]^{2}Σ^{+}(000) vibronic transitions. Molecules lost into the excited vibrational states during the cooling process are repumped back through the B[over ˜](000) state for both the (100) level of the Sr-O stretching mode and the (02^{0}0) level of the bending mode. The transverse temperature of a SrOH molecular beam is reduced in one dimension by 2 orders of magnitude to ∼750 µK. This approach opens a path towards creating a variety of ultracold polyatomic molecules by means of direct laser cooling.

Proposal for Laser Cooling of Complex Polyatomic Molecules.

An experimentally feasible strategy for direct laser cooling of polyatomic molecules with six or more atoms is presented. Our approach relies on the attachment of a metal atom to a complex molecule, where it acts as an active photon cycling site. We describe a laser cooling scheme for alkaline earth monoalkoxide free radicals taking advantage of the phase space compression of a cryogenic buffer-gas beam. Possible applications are presented including laser cooling of chiral molecules and slowing of molecular beams using coherent photon processes.

Reactions between layer-resolved molecules mediated by dipolar spin exchange.

Microscopic control over polar molecules with tunable interactions enables the realization of distinct quantum phenomena. Using an electric field gradient, we demonstrated layer-resolved state preparation and imaging of ultracold potassium-rubidium molecules confined to two-dimensional planes in an optical lattice. The rotational coherence was maximized by rotating the electric field relative to the light polarization for state-insensitive trapping. Spatially separated molecules in adjacent layers interact through dipolar spin exchange of rotational angular momentum; by adjusting these interactions, we regulated the local chemical reaction rate. The resonance width of the exchange process vastly exceeded the dipolar interaction energy, an effect attributed to thermal energy. This work realized precise control of interacting molecules, enabling electric field microscopy on subwavelength scales and allowing access to unexplored physics in two-dimensional systems.

Resonant collisional shielding of reactive molecules using electric fields.

Full control of molecular interactions, including reactive losses, would open new frontiers in quantum science. We demonstrate extreme tunability of ultracold chemical reaction rates by inducing resonant dipolar interactions by means of an external electric field. We prepared fermionic potassium-rubidium molecules in their first excited rotational state and observed a modulation of the chemical reaction rate by three orders of magnitude as we tuned the electric field strength by a few percent across resonance. In a quasi-two-dimensional geometry, we accurately determined the contributions from the three dominant angular momentum projections of the collisions. Using the resonant features, we shielded the molecules from loss and suppressed the reaction rate by an order of magnitude below the background value, thereby realizing a long-lived sample of polar molecules in large electric fields.

A degenerate Fermi gas of polar molecules.

Experimental realization of a quantum degenerate gas of molecules would provide access to a wide range of phenomena in molecular and quantum sciences. However, the very complexity that makes ultracold molecules so enticing has made reaching degeneracy an outstanding experimental challenge over the past decade. We now report the production of a degenerate Fermi gas of ultracold polar molecules of potassium-rubidium. Through coherent adiabatic association in a deeply degenerate mixture of a rubidium Bose-Einstein condensate and a potassium Fermi gas, we produce molecules at temperatures below 0.3 times the Fermi temperature. We explore the properties of this reactive gas and demonstrate how degeneracy suppresses chemical reactions, making a long-lived degenerate gas of polar molecules a reality.