Hybrid functionals for large periodic systems in an all-electron, numeric atom-centered basis framework

We describe a framework to evaluate the Hartree-Fock exchange operator for periodic electronic-structure calculations based on general, localized atom-centered basis functions. The functionality is demonstrated by hybrid-functional calculations of properties for several semiconductors. In our implementation of the Fock operator, the Coulomb potential is treated either in reciprocal space or in real space, where the sparsity of the density matrix can be exploited for computational efficiency. Computational aspects, such as the rigorous avoidance of on-the-fly disk storage, and a load-balanced parallel implementation, are also discussed. We demonstrate linear scaling of our implementation with system size by calculating the electronic structure of a bulk semiconductor (GaAs) with up to 1,024 atoms per unit cell without compromising the accuracy.

Duke Scholars

Author Volker Blum Thomas Lord Department of Mechanical Engineering and Materia ...