A Parameter-Free Reference Hamiltonian for Tight-Binding Vanadium Oxides
This paper introduces a parameter-free tight-binding reference Hamiltonian for vanadium oxides that overcomes the large, offsetting errors of standard second-order methods by deriving from superposed neutral atoms and full PBE potentials, thereby achieving high accuracy in energy differences and charge responses while clarifying that symmetry breaking in Magnéli phases requires explicit electron-lattice or spin-correlation terms.