Interpolative Separable Density Fitting Decomposition for Accelerating Hybrid Density Functional Calculations With Applications to Defects in Silicon

TL;DR

The paper introduces an efficient interpolative separable density fitting (ISDF) method combined with the ACE operator to significantly accelerate hybrid DFT calculations, enabling large-scale silicon defect simulations within minutes.

Contribution

It develops the ACE-ISDF approach that reduces computational cost of hybrid DFT, allowing large system simulations with high accuracy and scalability.

Findings

Reduces exchange operator computation from O(N_e^2) to O(N_e)

Achieves nearly two orders of magnitude speedup for large silicon systems

Enables hybrid DFT calculations on 1000-atom silicon within 10 minutes

Abstract

We present a new efficient way to perform hybrid density functional theory (DFT) based electronic structure calculation. The new method uses an interpolative separable density fitting (ISDF) procedure to construct a set of numerical auxiliary basis vectors and a compact approximation of the matrix consisting of products of occupied orbitals represented in a large basis set such as the planewave basis. Such an approximation allows us to reduce the number of Poisson solves from $\Or(N_{e}^2)$ to $\Or(N_{e})$ when we apply the exchange operator to occupied orbitals in an iterative method for solving the Kohn-Sham equations, where $N_{e}$ is the number of electrons in the system to be studied. We show that the ISDF procedure can be carried out in $\Or(N_{e}^3)$ operations, with a much smaller pre-constant compared to methods used in existing approaches. When combined with the recently developed adaptively compressed exchange (ACE) operator formalism, which reduces the number of times the exchange operator needs to be updated, the resulting ACE-ISDF method significantly reduces the computational cost \REV{associated with the exchange operator} by nearly two orders of magnitude compared to existing approaches for a large silicon system with $1000$ atoms. We demonstrate that the ACE-ISDF method can produce accurate energies and forces for insulating and metallic systems, and that it is possible to obtain converged hybrid functional calculation results for a 1000-atom bulk silicon within 10 minutes on 2000 computational cores. We also show that ACE-ISDF can scale to 8192 computational cores for a 4096-atom bulk silicon system. We use the ACE-ISDF method to geometrically optimize a 1000-atom silicon system with a vacancy defect using the HSE06 functional and computes its electronic structure.