Pyroelectric‐Accelerated Perovskite Photodetector for Picosecond Light Detection and Ranging

Abstract Light detection and ranging (LiDAR) is indispensable in applications such as unmanned aerial vehicles, autonomous driving, and biomimetic robots. However, the precision and available distance of LiDAR are constrained by the speed and sensitivity of the photodetector, necessitating the use of expensive and energy‐consuming avalanche diodes. To address these challenges, in this study, a pyroelectricity‐based acceleration strategy with 2D‐(graded 3D) perovskite heterojunction is proposed to achieve a record high speed (27.7 ns with an active area of 9 mm², and 176 ps with an active area of 0.2 mm²) and high responsivity (0.65 A W⁻¹) at zero bias. This success is attributed to the unique mechanism where the electrons from the pyroelectric effect at the Cl‐rich 2D/3D interface directly recombine with excess holes during light–dark transitions, breaking speed limitations related to carrier mobility and capacitive effect. Furthermore, the introduced pyroelectric effect significantly enhances the photoresponse, resulting in a self‐powered external quantum efficiency exceeding 100%. The study also demonstrates precise position detection at the centimeter level. In conclusion, this research presents a pioneering approach for developing high‐speed photodiodes with exceptional sensitivity, mitigating energy and cost concerns in LiDAR applications.