RT Journal Article SR Electronic T1 Accessing new magnetic regimes by tuning the ligand spin-orbit coupling in van der Waals magnets JF Science Advances JO Sci Adv FD American Association for the Advancement of Science SP eabb9379 DO 10.1126/sciadv.abb9379 VO 6 IS 30 A1 Tartaglia, Thomas A. A1 Tang, Joseph N. A1 Lado, Jose L. A1 Bahrami, Faranak A1 Abramchuk, Mykola A1 McCandless, Gregory T. A1 Doyle, Meaghan C. A1 Burch, Kenneth S. A1 Ran, Ying A1 Chan, Julia Y. A1 Tafti, Fazel YR 2020 UL http://advances.sciencemag.org/content/6/30/eabb9379.abstract AB 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 − x − yBrxIy, 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 − x − yBrxIy crystals at the same field as in the exfoliation experiments.