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Van der Waals (VdW) materials have opened new directions in the study of lowdimensional magnetism. A largely unexplored arena is the intrinsic tuning ofVdW magnets toward new ground-states. The chromium trihalides provided thefirst such example with a change of inter-layer magnetic coupling emerging uponexfoliation. Here, we take a different approach to engineer new ground-states,not by exfoliation, but by tuning the spin-orbit coupling (SOC) of thenon-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 functionof Cl, Br, and I content. The resulting triangular phase diagrams unveil afrustrated regime near CrCl$_{3}$. First-principles calculations confirm thatthe frustration is driven by a competition between the chromium and halideSOCs. Furthermore, we reveal a field-induced change of inter-layer coupling inthe bulk of CrCl$_{3-x-y}$Br$_{x}$I$_{y}$ crystals at the same field as in theexfoliation experiments.

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