Tuning magnetic and transport properties in quasi-2D (Mn_(1-x)Ni_x)₂P₂S₆ single crystals

We report an optimized chemical vapor transport method to grow single crystals of (Mn$_{1-x}$Ni$_x$)$_2$P$_2$S$_6$ where x = 0, 0.3, 0.5, 0.7 & 1. Single crystals up to 4\,mm\,$\times$\,3\,mm\,$\times$\,200\,$\mu$m were obtained by this method. As-grown crystals characterized by means of scanning electron microscopy, and powder x-ray diffraction measurements. The structural characterization shows that all crystals crystallize in monoclinic symmetry with the space group $C2/m$ (No. 12). We have further investigated the magnetic properties of this series of single crystals. The magnetic measurements of the all as-grown single crystals show long-range antiferromagnetic order along all crystallographic principal axes. Overall, the N\'eel temperature TN is non-monotonous, with increasing $Ni^{2+}$ doping the temperature of the antiferromagnetic phase transition first decreases from 80 K for pristine Mn$_2$P$_2$S$_6$ (x = 0) up to x = 0.5, and then increases again to 155 K for pure Ni$_2$P$_2$S$_6$ (x = 1). The magnetic anisotropy switches from out-of-plane to in-plane as a function of composition in (Mn$_{1-x}$Ni$_x$)$_2$P$_2$S$_6$ series. Transport studies under hydrostatic pressure on the parent compound Mn$_2$P$_2$S$_6$ evidence an insulator-metal transition at an applied critical pressure of ~22 GPa