Next, we perform DeePMD simulations to investigate the correlative dynamics between the Co ion migrations and the oxygen dimer formation. Similarly, we construct a DP model using the concurrent learning process (see Figure ). Here we briefly explain the difference in the DP construction workflow of this section from that employed in the above bulk LixCoO2 DP model training. First, since a reliable initial dataset could accelerate the convergence of the concurrent learning process, the CI-NEB method combined with structural perturbations are used to sample the initial dataset. Second, the metadynamics method, one of the enhanced sampling techniques, is introduced during the configurational exploration stage. The reason for employing the enhanced sampling approach is that the system's structure will rapidly relax to local minima without an artificial bias in the MD simulations even if the initial configuration is close to the transition state, resulting in an inefficient sampling of the structures along the reaction path. With a converged DP model, we then use the moving restraint method to drive the Co migration in DeePMD simulations. Please refer to the SI methodology for the computational details about these two enhanced sampling techniques and the CV setup.