Systematic derivation of realistic spin-models for beyond-Heisenberg solids

TL;DR

This paper systematically derives realistic spin-model Hamiltonians from multi-orbital Hubbard models, revealing significant multi-spin interactions beyond the Heisenberg model, with implications for understanding magnetic properties of materials.

Contribution

It introduces a systematic method to derive low-energy spin Hamiltonians including multi-spin interactions from multi-orbital Hubbard models.

Findings

Biquadratic, three-spin, and four-spin interactions are significant for spin S≥1.

Three-spin interactions can be comparable to Heisenberg exchange in real materials.

The derived models improve understanding of magnetic spectra in complex solids.

Abstract

We present a systematic derivation of effective lattice spin Hamiltonians derived from a rotationally invariant multi-orbital Hubbard model including a term ensuring Hund's rule coupling. The Hamiltonians are derived down-folding the fermionic degrees of freedom of the Hubbard model into the proper low-energy spin sector using L\"owdin partitioning, which will be outlined in detail for the case of two sites and two orbitals at each site. Correcting the ground state systematically up to fourth order in the hopping of electrons, we find for spin $S\geq 1$ a biquadratic, three-spin and four-spin interaction beyond the conventional Heisenberg term. Comparing the puzzling energy spectrum of the magnetic states for a single Fe monolayer on Ru(0001), obtained from density functional theory, with the spin Hamiltonians taken at the limit of classical spins, we show that the previously ignored three-spin interaction can be comparable in size to the conventional Heisenberg exchange.