Non-coplanar helimagnetism in the layered van-der-Waals metal DyTe$_3$

Abstract

Magnetic materials with highly anisotropic chemical bonding can be exfoliated to realize ultrathin sheets or interfaces with highly controllable optical or spintronics responses, while also promising novel cross-correlation phenomena between electric polarization and the magnetic texture. The vast majority of these van-der-Waals magnets are collinear ferro-, ferri-, or antiferromagnets, with a particular scarcity of lattice-incommensurate helimagnets of defined left- or right-handed rotation sense, or helicity. Here we use polarized neutron scattering to reveal cycloidal, or conical, magnetic structures in DyTe$_3$, with coupled commensurate and incommensurate order parameters, where covalently bonded double-slabs of dysprosium square nets are separated by highly metallic tellurium layers. Based on this ground state and its evolution in a magnetic field as probed by small-angle neutron scattering (SANS), we establish a one-dimensional spin model with off-diagonal on-site terms, spatially modulated by the unconventional charge order in DyTe$_3$. The CDW-driven term couples to antiferromagnetism, or to the net magnetization in applied magnetic field, and creates a complex magnetic phase diagram indicative of competing interactions in an easily cleavable helimagnet. Our work paves the way for twistronics research, where helimagnetic layers can be combined to form complex spin textures on-demand, using the vast family of rare earth chalcogenides and beyond.