Evaluating Predicted Densities, Hamiltonians, and Density Matrices as Periodic SCF Initializers

Learned electronic states are usually evaluated by prediction error, even though their intended use is to accelerate the self-consistent-field (SCF) loop of density functional theory (DFT). We ask whether lower offline error actually yields a better SCF initializer. We construct $ρ$HD-43K, a 43,851-