Research ArticleCONDENSED MATTER PHYSICS

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

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Science Advances  24 Jul 2020:
Vol. 6, no. 30, eabb9379
DOI: 10.1126/sciadv.abb9379

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. Chromium trihalides provided the first such example with a change of interlayer magnetic coupling emerging upon exfoliation. Here, we take a different approach to engineer previously unknown ground states, not by exfoliation, but by tuning the spin-orbit coupling (SOC) of the nonmagnetic ligand atoms (Cl, Br, I). We synthesize a three-halide series, CrCl3 − xyBrxIy, and map their magnetic properties as a function of Cl, Br, and I content. The resulting triangular phase diagrams unveil a frustrated regime near CrCl3. 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 interlayer coupling in the bulk of CrCl3 − xyBrxIy crystals at the same field as in the exfoliation experiments.

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