Accurate, Large-Scale and Affordable Hybrid-PBE0 Calculations with GPU-Accelerated Supercomputers

Abstract

Performing high accuracy hybrid functional calculations for condensed matter systems containing a large number of atoms is at present computationally very demanding - when not out of reach - if high quality basis sets are used. We present a highly efficient multiple GPU implementation of the exact exchange operator which allows hybrid functional density-functional theory calculations with systematic basis sets without additional approximations for up to a thousand atoms. This method is implemented in a portable real-space-based algorithm, released as an open-source package. With such a framework hybrid DFT calculations of high quality become accessible on state-of-the-art supercomputers within a time-to-solution of the same order of magnitude as traditional semilocal-GGA functionals.