Tucker tensor approach for accelerating exchange computations in a real-space finite-element discretization of generalized Kohn-Sham density functional theory

Abstract

The evaluation of Fock exchange is often the computationally most expensive part of hybrid functional density functional theory calculations in a systematically improvable, complete basis. In this work, we employ a Tucker tensor based approach that substantially accelerates the evaluation of the action of Fock exchange by transforming 3-dimensional convolutional integrals into a tensor product of 1-dimensional convolution integrals. Our numerical implementation uses a parallelization strategy that balances the memory and communication bottlenecks, alongside overalapping compute and communication operations to enhance computational efficiency and parallel scalability. The accuracy and computational efficiency is demonstrated on various systems, including Pt clusters of various sizes and a $\text{TiO}_{\text{2}}$ cluster with 3,684 electrons.