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.
