Interfacial Hot-Hole Relaxation and Transfer Dynamics from Lead Halide Perovskite Nanocrystals to Corroles for...

Understanding the hot-carrier (HC) relaxation and interfacial transfer dynamics in lead halide perovskites is crucial for developing high-performance optoelectronic devices. Herein, we investigate the hot-hole relaxation and transfer from cesium lead bromide (CPB) to the corrole derivative (m-Cor) using femtosecond transient absorption spectroscopy (fs-TAS). Under above bandgap photoexcitation, the CPB/m-Cor heterostructure exhibits faster HC relaxation (∼270 fs), accompanied by narrowing of the high-energy bleach tail and reduced initial HC temperature compared to pristine CPB. These spectral signatures indicate efficient interfacial extraction of hot holes from CPB to m-Cor, which is supported by density functional theory (DFT) calculations. Furthermore, the perovskite photodetector incorporating m-Cor as the hole-transport layer (HTL) exhibits ∼56%, ∼57%, and ∼180% enhancement in photocurrent, detectivity, and responsivity, respectively. Our findings provide mechanistic insight into the interfacial hot-hole transfer in perovskite nanocrystals as well as highlight m-Cor as a promising hole-transport material for the development of efficient perovskite optoelectronics.