Exchange interactions and magnetic force theorem

TL;DR

This paper critically examines the theoretical foundations of interatomic exchange interactions, comparing the magnetic force theorem with exact formulations, and proposes improved methods for modeling magnetic systems across various materials.

Contribution

It clarifies the differences between the magnetic force theorem and exact theory, and introduces a simple downfolding procedure for ligand spin elimination in exchange interaction calculations.

Findings

MFT provides reasonable results in many cases but has limitations.

Exact formulations are more consistent for ligand treatment and spin rotations.

Proposed downfolding method effectively incorporates ligand effects.

Abstract

We critically reexamine the problem of interatomic exchange interactions, which describe the total energy change caused by infinitesimal rotations of spins near some equilibrium state. For the small variations, such interactions can be always related to the response function. However, the form of this relation can depend on additional approximations. Particularly, the commonly used magnetic force theorem (MFT) prescribes the linear relation between the exchange interactions and the response function, while the exact theory requires this dependence to be inverse. We explore the origin and consequences of these differences in the definition for the wide class of materials: ferromagnetic Ni, antiferromagnetic NiO, half-metallic CrO2, multiferroic HoMnO3, and layered magnets CrCl3 and CrI3. While in most of these cases, MFT produces quite reasonable results and can be rigorously justifies in the long wavelength and strong-coupling limits, the exact formulation appears to be more consistent, especially in dealing with two important issues, which typically arise in the theory of exchange interactions: (i) the treatment of the ligand states, and (ii) the choice of the suitable variable for the description of infinitesimal rotations of spins. Both issues can be efficiently resolved by employing the ideas of adiabatic spin dynamics supplemented with the exact expression for the exchange interactions. Particularly, we propose a simple "downfolding" procedure for the elimination of the ligand spins by transferring their effect to the interaction parameters between the localized spins. Furthermore, we argue that the rotations of spin moments are more suitable for the description of low-energy excitations, while the rotations of the whole magnetization matrix cause much stronger perturbation in the system of spins.