Radical n–p Conduction Switching and Significant Photoconductivity Enhancement in NbOI2 via Pressure-Modulated Peierls Distortion

The absence of intrinsic p-type 2D layered semiconductors has hampered the development of 2D devices, particularly in complementary metal–oxide–semiconductor (CMOS) devices and integrated circuits. Developing practical p-type semiconductors and advanced modulation techniques for precise carrier control is paramount to advancing electronic devices and systems. Here, by applying pressure to continuously tune the Peierls distortion in NbOI2, we effectively control the polarity and concentration of carriers and significantly enhance its photoelectric properties. The results demonstrate that by suppressing the off-center displacement of Nb atoms along the in-plane b direction under pressure, NbOI2 undergoes a semiconductor-to-semiconductor phase transition from C2 to C2/m, leading to a significant transition from n-type to p-type carrier behavior. Additionally, the gradual inhibition of internal interactions within Nb–Nb dimers along the in-plane c direction under high pressure facilitates electron delocalization, substantially enhancing the photoelectric properties. The photocurrent is increased by more than 3 orders of magnitude under xenon irradiation, and the spectral response range is continuously red-shifted and extended to 1450 nm. These findings highlight the potential of pressure engineering to adjust photoelectric properties effectively and flexibly, offering valuable insights for designing high-performance p-type two-dimensional semiconductors.