Pressure-induced photocurrent enhancement and metallization in van der Waals compound SiTe2

Layered van der Waals (vdW) dichalcogenides are distinguished by their unique crystal structures and high structural tunability, rendering them suitable for applications in optics and optoelectronics. Despite significant processes, some fundamental questions remain in two-dimensional (2D) vdW dichalcogenides, such as clarifying detailed structure–property relationship and further improving the optoelectronic performance. Herein, by applying pressure to tune the crystal structure in 2D vdW dichalcogenide SiTe2, we realized a five orders of magnitude boost in photocurrent at 8 GPa. Such an enhancement is attributed to bandgap narrowing and an increased carrier concentration. Furthermore, bandgap closing and metallization were observed at 15.4 GPa, further suggesting the significant change of electronic structure upon compression. This study not only elucidates the intriguing pressure-induced behavior of SiTe2 but also paves the way for harnessing the unique pressure-responsive properties of 2D vdW dichalcogenides in advanced optoelectronic systems.