Periodic Pulay method for robust and efficient convergence acceleration of self-consistent field iterations

TL;DR

This paper introduces a periodic Pulay method that enhances the robustness and efficiency of self-consistent field iterations in electronic structure calculations by performing Pulay extrapolation periodically instead of every iteration.

Contribution

A novel generalization of DIIS that applies Pulay extrapolation periodically, improving convergence stability and computational efficiency in density functional theory calculations.

Findings

Significantly improved robustness in convergence.

Enhanced efficiency over standard Pulay methods.

Effective across various materials systems.

Abstract

Pulay's Direct Inversion in the Iterative Subspace (DIIS) method is one of the most widely used mixing schemes for accelerating the self-consistent solution of electronic structure problems. In this work, we propose a simple generalization of DIIS in which Pulay extrapolation is performed at periodic intervals rather than on every self-consistent field iteration, and linear mixing is performed on all other iterations. We demonstrate through numerical tests on a wide variety of materials systems in the framework of density functional theory that the proposed generalization of Pulay's method significantly improves its robustness and efficiency.