Structural stability, band structure and magnetic properties of ZnS and Zn0.75Cr0.25S under pressure

► Zn0.75Cr0.25S is more anisotropic and is easier to deform than ZnS. ► ZnS can exist stably under pressure up to 10 GPa with increasing direct band gap. ► The structural stability can be kept up to 5 GPa for the case of Zn.075Cr0.25S. ► Zn.075Cr0.25S is half metallic with Eg and Eg-HM increasing with P below 6 GPa. ► Δx(d) and Δx(pd) decrease as pressure increases.