Stereochemically Active Lone Pair Induced Polar Tri‐layered Perovskite for Record‐Performance Polarized Photodetection

Bulk photovoltaic effect, a promising optoelectronic phenomenon for generating polarized dependent steady-state photocurrent, has been widely applied in various photodetectors. However, incorporating stereochemically active lone pair to construct bulk photovoltage in organic-inorganic hybrid perovskite (OIHP) is still elusive and challenging. Herein, bulk photovoltage (1.2 V) has been successfully achieved by introducing the stereo-chemically active lone pair perovskitizer to construct a polar tri-layered hybrid perovskite, namely, (IBA)2 MHy2 Pb3 Br10 (1, IBA=iso-butylamine, MHy=methylhydrazine). Strikingly, owning to the promising bulk photovoltage, 1-based detectors exhibit an ultra-highly sensitive polarized photodetection (polarization ratio of up to 24.6) under self-powered mode. This ratio surpasses all the reported two-dimension OIHP single-crystal photodetectors. In addition, detectors exhibit outstanding responsivity (≈200 mA W-1 ) and detectivity (≈2.4×1013 Jones). More excitingly, further investigation confirms that lone pair electrons in MHy+ result in the separation of positive and negative charges to produce directional dipoles, which further directional alignment to generate bulk photovoltage, thereby resulting in polarization-dependent photocurrent. Our findings provide a new demonstration for polar multilayer materials' construction and may open opportunities for a host of high-sensitive polarized photodetection.