Establishing magneto-structural relationships in the solid solutions of the skyrmion hosting family of materials: GaV₄S_(8-y)Se_(y)

The GaV$_4$S$_{8-y}$Se$_y$ $(y = 0$ to $8)$ family of materials have been synthesized in both polycrystalline and single crystal form, and their structural and magnetic properties thoroughly investigated. Each of these materials crystallizes in the $F\bar{4}3m$ space group at ambient temperature. However, in contrast to the end members GaV$_4$S$_8$ and GaV$_4$Se$_8$, that undergo a structural transition to the $R3m$ space group at 42 and 41 K respectively, the solid solutions $(y = 1$ to $7)$ retain cubic symmetry down to 1.5 K. In zero applied field the end members of the family order ferromagnetically at 13 K (GaV$_4$S$_8$) and 18 K (GaV$_4$Se$_8$), while the intermediate compounds exhibit a spin-glass-like ground state. We demonstrate that the magnetic structure of GaV$_4$S$_8$ shows localization of spins on the V cations, indicating that a charge ordering mechanism drives the structural phase transition. We conclude that the observation of both structural and ferromagnetic transitions in the end members of the series in zero field is a prerequisite for the stabilization of a skyrmion phase, and discuss how the absence of these transitions in the $y = 1$ to $7$ materials can be explained by their structural properties.