Suppression of ferromagnetism and emergence of spin-glass-like behavior in the CuCr2−xSnxS2Se2 spinels

Magnetometry, neutron diffraction experiments, and high-resolution transmission electron microscopy (HRTEM) were performed to study the magnetic behavior of ${\mathrm{CuCr}}_{2\ensuremath{-}x}{\mathrm{Sn}}_{x}{\mathrm{S}}_{2}{\mathrm{Se}}_{2}$ ($0.2\ensuremath{\le}x\ensuremath{\le}1.0$) solid solutions and experimentally determine the appropriate magnetic structure for these systems. For all samples, the main phase with normal spinel-type structure ($Fd\overline{3}m$) was refined. For low Sn concentration a minority monoclinic phase appears also corroborated with HRTEM analyses. Together with the results from magnetization experiments, neutron diffraction measurements allowed to establish that for samples with $x\ensuremath{\le}0.4$ there is a ferromagnetic long-range order at high temperatures labeled with the $3d$ irrep $\mathrm{m}{\mathrm{\ensuremath{\Gamma}}}_{4}^{+}$ of $Fd\overline{3}m.{1}^{\ensuremath{'}}$, while for $x>0.4$ no magnetic signal is observed, indicating that the ferromagnetic behavior is suppressed and replaced with a spin-glass-like state.