Ab initio determination of spin Hamiltonians with anisotropic exchange interactions: the case of the pyrochlore ferromagnet Lu$_2$V$_2$O$_7$

TL;DR

This paper introduces a comprehensive ab initio framework for deriving effective spin Hamiltonians with anisotropic exchange interactions, demonstrated on the pyrochlore Lu$_2$V$_2$O$_7$, capturing key magnetic interactions and comparing with experiments.

Contribution

The paper develops a novel method combining DFT, Hubbard model diagonalization, and spin projections to accurately determine anisotropic exchange interactions in magnetic materials.

Findings

Quantitative estimates of exchange interactions in Lu$_2$V$_2$O$_7$

Identification of the role of Dzyaloshinskii-Moriya interactions

Agreement with experimental magnetic data

Abstract

We present a general framework for deriving effective spin Hamiltonians of correlated magnetic systems based on a combination of relativistic ab initio density functional theory calculations (DFT), exact diagonalization of a generalized Hubbard Hamiltonian on finite clusters and spin projections onto the low-energy subspace. A key motivation is to determine anisotropic bilinear exchange couplings in materials of interest. As an example, we apply this method to the pyrochlore Lu$_2$V$_2$O$_7$ where the vanadium ions form a lattice of corner-sharing spin-1/2 tetrahedra. In this compound, anisotropic Dzyaloshinskii-Moriya interactions (DMI) play an essential role in inducing a magnon Hall effect. We obtain quantitative estimates of the nearest-neighbor Heisenberg exchange, the DMI, and the symmetric part of the anisotropic exchange tensor. Finally, we compare our results with experimental ones on the Lu$_2$V$_2$O$_7$ compound.