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

TL;DR

This paper introduces a GPU-accelerated, open-source implementation of hybrid functional calculations in density-functional theory, enabling high-accuracy simulations of large condensed matter systems efficiently on supercomputers.

Contribution

It presents a novel, scalable GPU-based method for hybrid DFT calculations that handles systems with up to a thousand atoms without approximations.

Findings

Achieves hybrid DFT calculations comparable in speed to semilocal-GGA methods.

Supports systematic basis sets for high-accuracy results.

Open-source implementation enhances accessibility and reproducibility.

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.