Pressure-induced metallization in the absence of a structural transition in the layered ferromagnetic insulator Cr2Ge2Te6

We report the crystallographic and electrical transport properties of single crystals of the ferromagnetic two-dimensional (2D) material ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$ under high pressure. In contrast to previous studies, our high-pressure single-crystal x-ray diffraction under hydrostatic conditions shows prominent anisotropic compressibility in the layered structure of the crystalline $R\overline{3}$ phase of ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$ without any structural phase transitions up to 20 GPa. Our data confirm a distinct and irreversible crystalline-amorphous transformation in ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$. The loss of crystallinity starts at 20 GPa; however, the crystalline phase and amorphous state coexist even at the maximum pressure of 31.2 GPa. High-pressure powder x-ray diffraction data and electrical resistivity measurements of ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$ using NaCl as the pressure-transmitting medium reveal an insulator-to-metal transition in the absence of a phase transition at \ensuremath{\sim}3.9 GPa; at a considerably lower pressure than the previously reported (7--14 GPa). Density functional theory calculations demonstrate the density of states around the Fermi level are primarily dominated by Cr $3d$ and Te $5p$ states. Hence the large reduction of Cr-Te bond lengths within the ${\mathrm{CrTe}}_{6}$ octahedra under compression is most likely responsible for the band-gap closure. This study clarifies that the phase stability and onset of metallization pressure in the ${\mathrm{Cr}}_{2}{\mathrm{Ge}}_{2}{\mathrm{Te}}_{6}$ sample are sensitive to the hydrostatic environments and demonstrates how pressure can be used to tune the physical properties of 2D ferromagnetic compounds.