First-principle studies of the spin-orbit and the Dzyaloshinskii-Moriya interactions in the \{Cu$_3$\} single-molecule magnet

TL;DR

This study uses first-principles calculations and a Hubbard model approach to analyze how spin-orbit interaction influences the Dzyaloshinskii-Moriya interaction and chiral states in the Cu3 single-molecule magnet, providing insights into microscopic interactions.

Contribution

It introduces a Hubbard model-based method to connect spin-orbit interaction with the Dzyaloshinskii-Moriya interaction from first-principles calculations.

Findings

The ground-state splitting is approximately 0.02 meV, aligning with experimental data.

The Hubbard model yields improved estimates of the isotropic exchange constant.

The Dzyaloshinskii-Moriya interaction originates from off-diagonal spin-orbit interactions.

Abstract

Frustrated triangular molecule magnets such as \{Cu$_3$\} are characterized by two degenerate S=1/2 ground-states with opposite chirality. Recently it has been proposed theoretically [PRL {\bf 101}, 217201 (2008)] and verified by {\it ab-initio} calculations [PRB {\bf 82}, 155446 (2010)] that an external electric field can efficiently couple these two chiral spin states, even in the absence of spin-orbit interaction (SOI). The SOI is nevertheless important, since it introduces a splitting in the ground-state manifold via the Dzyaloshinskii-Moriya interaction. In this paper we present a theoretical study of the effect of the SOI on the chiral states within spin density functional theory. We employ a recently-introduced Hubbard model approach to elucidate the connection between the SOI and the Dzyaloshinskii-Moriya interaction. This allows us to express the Dzyaloshinskii-Moriya interaction constant $D$ in terms of the microscopic Hubbard model parameters, which we calculate from first-principles. The small splitting that we find for the \{Cu$_3$\} chiral state energies ($\Delta \approx 0.02$ meV) is consistent with experimental results. The Hubbard model approach adopted here also yields a better estimate of the isotropic exchange constant than the ones obtained by comparing total energies of different spin configurations. The method used here for calculating the DM interaction unmasks its simple fundamental origin which is the off-diagonal spin-orbit interaction between the generally multireference vacuum state and single-electron excitations out of those states.