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Structural evolution and bandgap modulation of layered β-GeSe2 single crystal under high pressure

Germanium diselenide (GeSe2) is a promising candidate for electronic devices because of its unique crystal structure and optoelectronic properties. However, the evolution of lattice and electronic structure of β-GeSe2 at high pressure is still uncertain. Here we prepared high-quality β-GeSe2 single crystals by chemical vapor transfer (CVT) technique and performed systematic experimental studies on the evolution of lattice structure and bandgap of β-GeSe2 under pressure. High-precision high-pressure ultra low frequency (ULF) Raman scattering and synchrotron angle-dispersive x-ray diffraction (ADXRD) measurements support that no structural phase transition exists under high pressure up to 13.80 GPa, but the structure of β-GeSe2 turns into a disordered state near 6.91 GPa and gradually becomes amorphous forming an irreversibly amorphous crystal at 13.80 GPa. Two Raman modes keep softening abnormally upon pressure. The bandgap of β-GeSe2 reduced linearly from 2.59 eV to 1.65 eV under pressure with a detectable narrowing of 36.5%, and the sample under pressure performs the piezochromism phenomenon. The bandgap after decompression is smaller than that in the atmospheric pressure environment, which is caused by incomplete recrystallization. These results enrich the insight into the structural and optical properties of β-GeSe2 and demonstrate the potential of pressure in modulating the material properties of two-dimensional (2D) Ge-based binary material.