Two-dimensional ferromagnetic superlattices

Abstract

Mechanically exfoliated two-dimensional ferromagnetic materials (2D FMs) possess long-range ferromagnetic order and topologically nontrivial skyrmions in few layers. However, because of the dimensionality effect, such few-layer systems usually exhibit much lower Curie temperature (<i>T</i> _C) compared to their bulk counterparts. It is therefore of great interest to explore effective approaches to enhance their <i>T</i> _C, particularly in wafer-scale for practical applications. Here, we report an interfacial proximity-induced high-<i>T</i> _C 2D FM Fe₃GeTe₂ (FGT) via A-type antiferromagnetic material CrSb (CS) which strongly couples to FGT. A superlattice structure of (FGT/CS)_n, where <i>n</i> stands for the period of FGT/CS heterostructure, has been successfully produced with sharp interfaces by molecular-beam epitaxy on 2-inch wafers. By performing elemental specific X-ray magnetic circular dichroism (XMCD) measurements, we have unequivocally discovered that <i>T</i> _C of 4-layer Fe₃GeTe₂ can be significantly enhanced from 140 K to 230 K because of the interfacial ferromagnetic coupling. Meanwhile, an inverse proximity effect occurs in the FGT/CS interface, driving the interfacial antiferromagnetic CrSb into a ferrimagnetic state as evidenced by double-switching behavior in hysteresis loops and the XMCD spectra. Density functional theory calculations show that the Fe-Te/Cr-Sb interface is strongly FM coupled and doping of the spin-polarized electrons by the interfacial Cr layer gives rise to the <i>T</i> _C enhancement of the Fe₃GeTe₂ films, in accordance with our XMCD measurements. Strikingly, by introducing rich Fe in a 4-layer FGT/CS superlattice, <i>T</i> _C can be further enhanced to near room temperature. Our results provide a feasible approach for enhancing the magnetic order of few-layer 2D FMs in wafer-scale and render opportunities for realizing realistic ultra-thin spintronic devices.