Microscopy of correlated dynamics using Rydberg macrodimers

Exciting atoms in optical lattices to Rydberg states enhances the cold atom toolbox by extended range interactions. Rydberg macrodimers - electrostatically bound Rydberg atom pairs - provide huge bond lengths larger than the typical distance between neighboring lattice sites. Combined with quantum gas microscopy, this allows us to measure how their photoassociation depends on the angle between the molecular axis and external control fields. The observed dependencies represent a fingerprint of the electronic structure and reveal the underlying molecular quantum numbers. Off-resonant coupling to macrodimers also opens new avenues to Rydberg-dressed interactions in the ground state manifold. We verify the presence of the engineered Ising Hamiltonian induced by dressing to macrodimer states by observing correlated spin flips at the molecular bond length using many-body Ramsey interferometry. Tuning the laser on resonance, we observe a spatial blockade mechanism between pairs of macrodimers arising from a combination of dipolar interactions between Rydberg atoms and macrodimers and macrodimer pairs. Our results represent the first quantum simulation based on Rydberg macrodimers and provide a new pathway to enter a correlated regime using Rydberg interactions.