Many-body models for molecular nanomagnets

TL;DR

This paper introduces a versatile ab-initio method using localized orbitals to model molecular nanomagnets, accurately calculating magnetic interactions and matching experimental results for various systems.

Contribution

The paper presents a new ab-initio scheme employing Foster-Boys orbitals for modeling magnetic properties of nanomagnets, demonstrating its effectiveness on multiple systems.

Findings

Accurately calculates magnetic exchange couplings and zero-field splittings.

Achieves excellent agreement with experimental data.

Identifies essential magnetic interactions in studied systems.

Abstract

We present a flexible and effective ab-initio scheme to build many-body models for molecular nanomagnets, and to calculate magnetic exchange couplings and zero-field splittings. It is based on using localized Foster-Boys orbitals as one-electron basis. We apply this scheme to three paradigmatic systems, the antiferromagnetic rings Cr8 and Cr7Ni and the single molecule magnet Fe4. In all cases we identify the essential magnetic interactions and find excellent agreement with experiments.