Cr₂Ge₂Te₆ is a rare layered ferromagnetic semiconductor that represents a promising material for novel thermoelectric and spintronic devices. High pressure is an effective way to change the electronic structure, and profoundly affects the physical and chemical properties of two-dimensional (2D) layered materials. Here we combined experimental results and theoretical calculations to investigate the structural evolution and properties of Cr₂Ge₂Te₆under high pressure. It is found that Cr₂Ge₂Te₆ undergoes an isostructural phase transition from layered to non-layered structure at ~14 GPa, accompanied with a semiconductor to metal transition, which is distinct from the previous reports. The pressure-induced metallization is verified by the overlap of the valence and conduction bands, and the layered-to-non-layered isostructural transition is attributed to the enhanced interlayer Te–Te interaction by First-principles calculations. Our results provide a potential pathway to control the structure and property of layered materials and possibility for conceptually new devices via pressure engineering.

Cr ₂ Ge ₂ Te ₆是一种稀有的层状铁磁半导体，代表了用于新型热电和自旋电子器件的有前途的材料。高压是改变电子结构的有效方法，并且深刻影响二维（2D）层状材料的物理和化学性质。在这里，我们结合实验结果和理论计算来研究Cr ₂ Ge ₂ Te ₆在高压下的结构演变和性能。发现Cr ₂ Ge ₂ Te ₆在〜14 GPa处经历了从分层结构到非分层结构的同构相变，并伴随着半导体到金属的转变，这与以前的报道不同。价位和导带的重叠验证了压力诱导的金属化，并且通过第一性原理计算，层到非层的同构过渡归因于增强的层间Te-Te相互作用。我们的结果提供了控制分层材料的结构和性能的潜在途径，以及通过压力工程为概念上新设备提供可能性的途径。