Two-axis twisting using Floquet-engineered XYZ spin models with polar molecules.

Polar molecules confined in an optical lattice are a versatile platform to explore spin-motion dynamics based on strong, long-range dipolar interactions1,2. The precise tunability3 of Ising and spin-exchange interactions with both microwave and d.c. electric fields makes the molecular system particularly suitable for engineering complex many-body dynamics4-6. Here we used Floquet engineering7 to realize new quantum many-body systems of polar molecules. Using a spin encoded in the two lowest rotational states of ultracold 40K87Rb molecules, we mutually validated XXZ spin models tuned by a Floquet microwave pulse sequence against those tuned by a d.c. electric field through observations of Ramsey contrast dynamics. This validation sets the stage for the realization of Hamiltonians inaccessible with static fields. In particular, we observed two-axis twisting8 mean-field dynamics, generated by a Floquet-engineered XYZ model using itinerant molecules in two-dimensional layers. In the future, Floquet-engineered Hamiltonians could generate entangled states for molecule-based precision measurement9 or could take advantage of the rich molecular structure for quantum simulation of multi-level systems10,11.

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.

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.