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

See allHide authors and affiliations

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


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.

This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

View Full Text

Stay Connected to Science Advances