Realistic non-collinear ground states of solids with source-free exchange correlation functional

TL;DR

This paper extends a source-free exchange-correlation functional to plane-wave DFT with PAW, demonstrating improved convergence and better agreement with experimental magnetic ground states, and analyzing the role of probability currents and XC torque.

Contribution

It introduces a source-free XC functional into plane-wave DFT with PAW, improving magnetic state predictions and analyzing spin-current effects.

Findings

Enhanced convergence behavior with the source-free functional.

Better agreement with experimental magnetic ground states.

Highlighted importance of probability currents and XC torque in spin systems.

Abstract

In this work, we extend the source-free (SF) exchange correlation (XC) functional developed by Sangeeta Sharma and co-workers to plane-wave density functional theory (DFT) based on the projector augmented wave (PAW) method. This constraint is implemented by the current authors within the VASP source code, using a fast Poisson solver that capitalizes on the parallel three-dimensional fast Fourier transforms (FFTs) implemented in VASP. Using this modified XC functional, we explore the improved convergence behavior that results from applying this constraint to the GGA-PBE+$U$+$J$ functional. In the process, we compare the non-collinear magnetic ground state computed by each functional and their SF counterpart for a select number of magnetic materials in order to provide a metric for comparing with experimentally determined magnetic orderings. We observe significantly improved agreement with experimentally measured magnetic ground state structures after applying the source-free constraint. Furthermore, we explore the importance of considering probability current densities in spin polarized systems, even under no applied field. We analyze the XC torque as well, in order to provide theoretical and computational analyses of the net XC magnetic torque induced by the source-free constraint. Along these lines, we highlight the importance of properly considering the real-space integral of the source-free local magnetic XC field. Our analysis on probability currents, net torque, and constant terms draws additional links to the rich body of previous research on spin-current density functional theory (SCDFT), and paves the way for future extensions and corrections to the SF corrected XC functional.