Boosting the Performance of Photomultiplication‐Type Organic Photodiodes by Embedding CsPbBr3 Perovskite Nanocrystals

In this study, it is demonstrated that CsPbBr3 perovskite nanocrystals (NCs) can enhance the overall performances of photomultiplication‐type organic photodiodes (PM‐OPDs). The proposed approach enables the ionic‐polarizable CsPbBr3 NCs to be evenly distributed throughout the depletion region of Schottky junction interface, allowing the entire trapped electrons within the depletion region to be stabilized, in contrast to previously reported interface‐limited strategies. The optimized CsPbBr3‐NC‐embedded poly(3‐hexylthiophene‐diyl)‐based PM‐OPDs exhibit exceptionally high external quantum efficiency, specific detectivity, and gain–bandwidth product of 2,840,000%, 3.97 × 1015 Jones, and 2.14 × 107 Hz, respectively. 2D grazing‐incidence X–ray diffraction analyses and drift–diffusion simulations combined with temperature‐dependent J–V characteristic analyses are conducted to investigate the physics behind the success of CsPbBr3‐NC‐embedded PM‐OPDs. The results show that the electrostatic interactions generated by the ionic polarization of NCs effectively stabilize the trapped electrons throughout the entire volume of the photoactive layer, thereby successfully increasing the effective energy depth of the trap states and allowing efficient PM mechanisms. This study demonstrates how a hybrid‐photoactive‐layer approach can further enhance PM‐OPD when the functionality of inorganic inclusions meets the requirements of the target device. A hybrid approach of embedding perovskite nanocrystals (NCs) into photoactive layers of photomultiplication‐type organic photodiodes (PM‐OPDs) is proposed. Embedded perovskite NCs polarize via migration of their constituting ions in the presence of an external applied bias and supply electrostatic interactions to trapped electrons over the entire volume of the photoactive layer, thereby resulting in ultrahigh performances of the optimized PM‐OPD.