Communication: comparing ab initio methods of obtaining effective U parameters for closed-shell materials.
The density functional theory (DFT)+U method is an efficient and effective way to calculate the ground-state properties of strongly correlated transition metal compounds, with the effective U parameters typically determined empirically. Two ab initio methods have been developed to compute the U parameter based on either constrained DFT (CDFT) or unrestricted Hartree-Fock (UHF) theory. Previous studies have demonstrated the success of both methods in typical open-shell materials such as FeO and NiO. In this Communication we report numerical instability issues that arise for the CDFT method when applied to closed-shell transition metals, by using ZnO and Cu2O as examples. By contrast, the UHF method behaves much more robustly for both closed- and open-shell materials, making it more suitable for treating closed-shell transition metals, as well as main group elements.
Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, New Jersey 08544-5263, USA.
Kuang
K
Yu
Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, New Jersey 08544-5263, USA.
Emily A
EA
Carter