Nonlocal pseudopotential energy density functional for semiconductors

Due to the linear scaling of the computational cost with system size, orbital-free density functional theory (OF-DFT) offers a promising approach for large-scale materials simulations. However, the lack of high transferability local pseudopotentials in OF-DFT has impeded its wide use for materials simulations. Recently, the nonlocal pseudopotential energy density functional (NLPPF) method [Nat. Commun. 13, 1385 (2022)] has been proposed to enable OF-DFT to directly use nonlocal pseudopotentials and successfully applied to simple metallic systems formed by sp-block metallic elements. Here, we extend the NLPPF scheme for applications to the semiconducting systems by employment of the revised Huang-Carter kinetic-energy density functional. Applications of typical semiconductors including Si, Ge, and GaAs have systematically benchmarked the scheme. The results demonstrate that the NLPPF scheme combined with the revised Huang-Carter kinetic-energy density functional can significantly improve the accuracy of OF-DFT for simulating the semiconductors without extensive requirements of computational budget, which opens up new opportunities for OF-DFT applications to large-scale semiconducting systems.