Accessing new magnetic regimes by tuning the ligand spin-orbit coupling in van der Waals magnets

Abstract

Van der Waals (VdW) materials have opened new directions in the study of low dimensional magnetism. A largely unexplored arena is the intrinsic tuning of VdW magnets toward new ground-states. The chromium trihalides provided the first such example with a change of inter-layer magnetic coupling emerging upon exfoliation. Here, we take a different approach to engineer new ground-states, not by exfoliation, but by tuning the spin-orbit coupling (SOC) of the non-magnetic ligand atoms (Cl,Br,I). We synthesize a three-halide series, CrCl${}_{3-x-y}$Br${}_x$I${}_y$, and map their magnetic properties as a function of Cl, Br, and I content. The resulting triangular phase diagrams unveil a frustrated regime near CrCl${}_3$. First-principles calculations confirm that the frustration is driven by a competition between the chromium and halide SOCs. Furthermore, we reveal a field-induced change of inter-layer coupling in the bulk of CrCl${}_{3-x-y}$Br${}_x$I${}_y$ crystals at the same field as in the exfoliation experiments.

22 pages, 6 figures

References in corpus (3)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Thermodynamic Evidence of Proximity to a Kitaev Spin-Liquid in Ag${}_3$LiIr${}_2$O${}_6$

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