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Long-range and anisotropic dipolar interactions profoundly modify the dynamics of particles hopping in a periodic lattice potential. Here, we report the realization of a generalized t-J model with dipolar interactions using a system of ultracold fermionic molecules with spin encoded in the two lowest rotational states. We systematically explore the role of dipolar Ising and spin-exchange couplings and the effect of motion on spin dynamics. The model parameters can be controlled independently, with dipolar couplings tuned by electric fields and motion regulated by optical lattices. Using Ramsey spectroscopy, we observed interaction-driven contrast decay that depends strongly both on the strength of the anisotropy between Ising and spin-exchange couplings and on motion. These observations are supported by theory models established in different motional regimes that provide intuitive pictures of the underlying physics. This study paves the way for future exploration of kinetic spin dynamics and quantum magnetism with highly tunable molecular platforms in regimes challenging for existing numerical and analytical methods, and it could shed light on the complex behaviors observed in real materials.

Polar molecules confined in an optical lattice are a versatile platform to explore spin-motion dynamics based on strong, long-range dipolar interactions. The precise tunability of Ising and spin-exchange interactions with both microwave and dc electric fields makes the molecular system particularly suitable for engineering complex many-body dynamics. Here, we used Floquet engineering to realize interesting quantum many-body systems of polar molecules. Using a spin encoded in the two lowest rotational states of ultracold KRb molecules, we mutually validated XXZ spin models tuned by a Floquet microwave pulse sequence against those tuned by a dc electric field through observations of Ramsey contrast dynamics, setting the stage for the realization of Hamiltonians inaccessible with static fields. In particular, we observed two-axis twisting mean-field dynamics, generated by a Floquet-engineered XYZ model using itinerant molecules in 2D layers. In the future, Floquet-engineered Hamiltonians could generate entangled states for molecule-based precision measurement or could take advantage of the rich molecular structure for quantum simulation of multi-level systems., Comment: 20 pages, 4 figures + 4 extended data figures

Strongly interacting spins underlie many intriguing phenomena and applications ranging from magnetism to quantum information processing. Interacting spins combined with motion display exotic spin transport phenomena, such as superfluidity arising from pairing of spins induced by spin attraction. 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 capabilities. 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 utilizing the strong, tunable dipolar interaction., Comment: 22 pages, including 4 + 2 figures

Microscopic control over polar molecules with tunable interactions would enable realization of novel quantum phenomena. Using an applied electric field gradient, we demonstrate layer-resolved state preparation and imaging of ultracold potassium-rubidium molecules confined to two-dimensional planes in an optical lattice. The coherence time of rotational superpositions in individual layers is maximized by rotating the electric field relative to the optical trap polarization to achieve state-insensitive trapping. Molecules in adjacent layers interact via dipolar exchange of rotational angular momentum; by adjusting the interaction strength between spatially separated ensembles of molecules, we regulate the local chemical reaction rate. The observed resonance width of the exchange process vastly exceeds the dipolar interaction energy, an effect we attribute to the thermal energy. This work realizes precise control of interacting molecules, enabling electric field microscopy on subwavelength length scales and allowing access to unexplored physics in two-dimensional systems., Comment: 20+8 pages, 4+4 figures