a1 Stanford University Department of Electrical Engineering, 350 Serra Mall Stanford, CA, U.S.A.
The structures and energies of stoichiometric and oxygen-deficient monoclinic HfO2 were calculated using density functional theory. The electronic interactions in HfO2 were calculated using the LDA+U and GGA+U formalisms, where on-site Coulomb corrections were applied to the 5d electrons of hafnium (U d ) and the 2p electrons of oxygen (U p ). Properties calculated using these techniques are compared to results obtained from LDA, GGA, hybrid functionals, and experiment. Ultimately, we show that LDA+U d +U p and GGA+U d +U p calculations of HfO2’s electronic and structural properties achieve a level of accuracy on par with much more computationally demanding hybrid functional techniques, such as PBE0 and HSE06.