Fast and scalable finite-element based approach for density functional theory calculations using projector-augmented wave method

Abstract

In this work, we present a computationally efficient methodology that utilizes a local real-space formulation of the projector augmented wave (PAW) method discretized with a finite-element (FE) basis to enable accurate and large-scale electronic structure calculations. To the best of our knowledge, this is the first real-space approach for DFT calculations, combining the efficiency of PAW formalism involving smooth electronic fields with the ability of systematically improvable higher-order finite-element basis to achieve significant computational gains. In particular, we have developed efficient strategies for solving the underlying FE discretized PAW generalized eigenproblem by employing the Chebyshev filtered subspace iteration approach to compute the desired eigenspace in each self-consistent field iteration. These strategies leverage the low-rank perturbation of the FE basis overlap matrix in conjunction with reduced order quadrature rules to invert the discretized PAW overlap matrix while also exploiting the sparsity of both the local and non-local parts of the discretized PAW Hamiltonian and overlap matrices. Using the proposed approach, we benchmark the accuracy and performance on various representative examples involving periodic and non-periodic systems with plane-wave-based PAW implementations. Furthermore, we also demonstrate a considerable computational advantage ($\sim$ 5$\times$ -- 10$\times$) over state-of-the-art plane-wave methods for medium to large-scale systems ($\sim$ 6,000 -- 35,000 electrons). Finally, we show that our approach (PAW-FE) significantly reduces the degrees of freedom to achieve the desired accuracy, thereby enabling large-scale DFT simulations ($>$ 50,000 electrons) at an order of magnitude lower computational cost compared to norm-conserving pseudopotential calculations using finite-element discretized calculations.