Short-range Crystalline Order-Tuned Conductivity in Cr${}_2$Si${}_2$Te${}_6$ van der Waals Magnetic Crystals

Two-dimensional magnetic materials (2DMM) are significant for studies on the nature of 2D long range magnetic order but also for future spintronic devices. Of particular interest are 2DMM where spins can be manipulated by electrical conduction. Whereas Cr${}_2$Si${}_2$Te${}_6$ exhibits magnetic order in few-layer crystals, its large band gap inhibits electronic conduction. Here we show that the defect-induced short-range crystal order in Cr${}_2$Si${}_2$Te${}_6$ on the length scale below 0.6 nm induces substantially reduced band gap and robust semiconducting behavior down to 2 K that turns to metallic above 10 GPa. Our results will be helpful to design conducting state in 2DMM and call for spin-resolved measurement of the electronic structure in exfoliated ultrathin crystals.