Self-consistent Gutzwiller study of bcc Fe: interplay of ferromagnetic order and kinetic energy

TL;DR

This study uses an ab-initio Gutzwiller+LDA approach to analyze ferromagnetism in bcc Fe, revealing that correlations cause a decrease in kinetic energy upon ferromagnetic ordering, contrary to previous models.

Contribution

It introduces a Gutzwiller+LDA method to accurately capture correlation effects in ferromagnetic bcc Fe, highlighting the role of orbital-specific behaviors and double exchange mechanisms.

Findings

Ferromagnetic order decreases kinetic energy in Fe due to correlations.

Orbital differentiation causes eg to localize and t2g to delocalize.

Double exchange mechanism is active in ferromagnetic Fe.

Abstract

The Gutzwiller technique has long been known as a method to include correlations in electronic structure calculations. Here we implement an ab-initio Gutzwiller+LDA calculation, and apply it to a classic problem, the ferromagnetism of bulk bcc Fe, whose nature has attracted recent interest. In the conventional Stoner-Wohlfarth model, the ferromagnetic ordering of iron sets in so that the electrons can reduce their mutual Coulomb repulsion at the extra cost of some increase of electron kinetic energy. Density functional theory within the spin polarized local density approximation (LDA) has long supported that picture, showing that ferromagnetic alignment causes band narrowing and a corresponding wavefunction localization, whence a kinetic energy increase. However, because of its inadequate treatment of strong intra-site correlations for localized d orbitals, LDA cannot be relied upon, particularly when it comes to separately describing fine potential and kinetic energy imbalances. With ab-initio Gutzwiller+LDA, we indeed find that the effect of correlations is to dramatically reverse the balance, the ferromagnetic ordering of Fe in fact causing a decrease of kinetic energy, at the cost of some increase of potential energy. The underlying physical mechanism, foreshadowed long ago by Goodenough and others, and more recently supported by LDA+DMFT calculations, is that correlations cause eg and t2g 3d orbitals to behave very differently. Weakly dispersive eg states are spin-polarized and almost localized, while, more than half filled, the t2g are broad band, fully delocalized states. Owing to intra-atomic Hund's rule exchange which aligns eg and t2g spins, the propagation of itinerant t2g holes is only allowed when different atomic spins are ferromagnetically aligned. We thus conclude that double exchange is at work already in the most popular ferromagnetic metal.