Long-range anisotropic Heisenberg ferromagnets and electrically tunable ordering

TL;DR

This paper develops a first-principles-based anisotropic Heisenberg model to accurately describe 2D magnetic materials, predicting electrical tuning of magnetic order and Curie temperature enhancements in chromium trihalides.

Contribution

It introduces a novel anisotropic Heisenberg model incorporating beyond-nearest-neighbor interactions, enabling quantitative predictions of magnetic properties and electrical tunability in 2D ferromagnets.

Findings

Accurately reproduces experimental magnetic behavior of chromium trihalides.

Predicts a five-fold increase in Curie temperature in monolayer CrI₃ via hole doping.

Demonstrates electrical doping, strain, and chemical doping effects on magnetic order.

Abstract

Recent realizations of intrinsic magnetic order in truly two-dimensional materials have opened new avenues in the fundamental knowledge and spintronic applications. Here we develop an anisotropic Heisenberg model with relativistic exchange interactions that are obtained from the first-principles calculations. We demonstrate the crucial importance of magnetic interactions beyond the first-neighbour to qualitatively and quantitatively reproduce the experimental results. Once we ascertain the predictive capacity of the model for chromium trihalides and CrGeTe$_3$, we investigate the feasibility of tuning the magnetic ordering by electrical means in these materials. A remarkable five-fold increase in the ferromagnetic Curie temperature is predicted in monolayer CrI$_3$ within experimentally obtainable hole density. The elusive microscopic mechanism behind the doping-dependent Curie temperature is illustrated. Further, in the present context, the effects of biaxial strain and chemical doping are also addressed. The results should trigger further experimental attention to test the present conclusions.