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Understanding quantum thermalization through entanglement build-up inisolated quantum systems addresses fundamental questions on how unitarydynamics connects to statistical physics. Here, we study the spin dynamics andapproach towards local thermal equilibrium of a macroscopic ensemble of S = 3spins prepared in a pure coherent spin state, tilted compared to the magneticfield, under the effect of magnetic dipole-dipole interactions. The experimentuses a unit filled array of 104 chromium atoms in a three dimensional opticallattice, realizing the spin-3 XXZ Heisenberg model. The buildup of quantumcorrelation during the dynamics, especially as the angle approaches pi/2, issupported by comparison with an improved numerical quantum phase-space methodand further confirmed by the observation that our isolated system thermalizesunder its own dynamics, reaching a steady state consistent with the oneextracted from a thermal ensemble with a temperature dictated from the system'senergy. This indicates a scenario of quantum thermalization which is tied tothe growth of entanglement entropy. Although direct experimental measurementsof the Renyi entropy in our macroscopic system are unfeasible, the excellentagreement with the theory, which can compute this entropy, does indicateentanglement build-up.

Exploring out-of-equilibrium quantum magnetism and thermalization in a spin-3 many-body dipolar lattice system