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Mixed halide chemistry has recently been utilized to tune the intrinsicmagnetic properties of transition-metal halides $-$ one of the largest familiesof magnetic van der Waals materials. Prior studies have shown that the strengthof exchange interactions, hence the critical temperature, can be tuned smoothlywith halide composition for a given ground-state. Here we show that theground-state itself can be altered by a small change of halide compositionleading to a quantum phase transition in FeCl$_{3-x}$Br$_x$. Specifically, wefind a three-fold jump in the N\'{e}el temperature and a sign change in theWeiss temperature at $x= 0.08$ corresponding to only $3\%$ bromine doping.Using neutron scattering, we reveal a change of the ground-state from spiralorder in FeCl$_3$ to A-type antiferromagnetic order in FeBr$_3$. Usingfirst-principles calculations, we show that a delicate balance between nearestand next-nearest neighbor interactions is responsible for such a transition.These results support the proximity of FeCl$_3$ to a spiral spin liquid state,in which competing interactions and nearly degenerate magnetic $k$-vectors maycause large changes in response to small perturbations.

Extreme sensitivity of the magnetic ground-state to halide composition in FeCl$_{3-x}$Br$_x$