2,2′,7,7′-Tetrakis-(N,N-di-p-methoxyphenyl-amine)-9,9′-spirobifluorene (spiro-OMeTAD) is one of the broadly used hole transport materials for high-performance perovskite photodetectors. However, to achieve high hole mobility and conductivity, it often requires the addition of additives and dopants with hygroscopic properties similar to bis(trifluoromethane)sulfonamide lithium salt (Li-TFSI) and 4-tert-butylpyridine (TBP), which are forced to undergo aggregation and hydrolysis under environmental conditions, hence leading to pinholes/voids in resultant films. In this work, we added rubidium iodide (RbI) to spiro-OMeTAD together with Li-TFSI and TBP, and the complexation between RbI and TBP prevented the evaporation of TBP that hinders the aggregation of Li-TFSI and reduces the undesired voids. Consequently, RbI-doped spiro-OMeTAD serves as the hole transport layer (HTL) for perovskite photodetectors, enhancing the conductivity and hole transport abilities of the hole transport layer, which also helps to promote energy-level matching with the perovskite layer. The performance of the perovskite photodetector is verified by analyzing the current density–voltage characteristics as well as the transient and dynamic photocurrent response characteristics. Devices with RbI-doped HTLs exhibit a champion specific detectivity approaching 3.77 × 1013 Jones and a linear dynamic range of 114 dB. This work provides a feasible approach to improve the stability of small-molecule-based hole transport materials for perovskite photodetectors.
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