Engineering Collinear Magnetization in Hexagonal LuFeO₃ and Magnetoelectric Control of Skyrmions in Hexagonal 2D Epilayers

Abstract

Cubic, perovskite‐structure ABO3‐ and A1−xA'xBO3‐type oxides have been investigated extensively while their hexagonal structure versions have not, even though they are multiferroic and can form heterostructures with hexagonal 2D materials. In particular, multiferroic 2D epilayers may lead to strong magnetoelectric coupling. Hexagonal RFeO3 ferrites, where R is a rare‐earth element (Lu, Yb, etc.), are excellent candidates, but their ferromagnetism is weak. In this work, density‐functional‐theory (DFT) calculations are employed and first show that heavy electron doping of hexagonal LuFeO3 (h‐LFO), namely Lu1−xHfxFeO3 (h‐LHFO), leads to spin‐disproportionation of the Fe sublattices and, especially for x = 1/2 and 2/3, to robust, room‐temperature, out‐of‐plane, collinear ferrimagnetism that is stabilized by a Jahn–Teller metal‐to‐insulator transition. h‐LHFO/h‐2D heterostructures are then shown, where h‐2D is the FE/FM monolayer MnSTe, to stabilize skyrmions without an external magnetic field and their chirality is controlled by an external electric field through the h‐LHFO polarization, opening up a new realm for magnetoelectric applications.