High‐Performance Photodetection of Quasi‐Two‐Dimensional Metal Halides for High‐Pressure Environments Enabled by Anti‐Wilson Effect

ABSTRACT Photodetectors are crucial for information acquisition in extreme high‐pressure environments. However, their performance is often limited by increased dark current and a reduced on/off ratio during compression. Here, we report a photodetector under high‐pressure based on EA 2 MA 2 Pb 3 Br 10 . Benefiting from anti‐Wilson effect, the device achieves a two‐order‐of‐magnitude suppression of dark current and a continuously improved on/off ratio under compression. At 23.6 GPa, it exhibits a responsivity of 1462.8 A W − 1 , the highest value yet reported for photodetectors under high‐pressure, together with an external quantum efficiency of 4.9 × 10 5 % and a detectivity of 6.1 × 10 13 Jones. Further studies reveal that pressure‐induced Pb–Br octahedral distortion drives the anti‐Wilson effect, while enhanced polarization increases the self‐powered photocurrent to 200% of its original value at 24.0 GPa. These results provide a new strategy for designing high‐performance self‐powered photodetectors for extreme environments.