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Rydberg atoms in optical lattices and tweezers is now a well establishedplatform for simulating quantum spin systems. However, the role of the atoms'spatial wavefunction has not been examined in detail experimentally. Here, weshow a strong spin-motion coupling emerging from the large variation of theinteraction potential over the wavefunction spread. We observe its clearsignature on the ultrafast, out-of-equilibrium, many-body dynamics of atomsexcited to a Rydberg S state from an unity-filling atomic Mott-insulator. Wealso propose a novel approach to tune arbitrarily the strength of thespin-motion coupling relative to the motional energy scale set by trappingpotentials. Our work provides a new direction for exploring the dynamics ofstrongly-correlated quantum systems by adding the motional degree of freedom tothe Rydberg simulation toolbox.

Strong Spin-Motion Coupling in the Ultrafast Quantum Many-body Dynamics of Rydberg Atoms in a Mott-insulator Lattice