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The anomalous photovoltaic (APV) effect in organic–inorganic hybrid perovskites (OIHPs) has attracted massive interest for developing high‐performance optoelectronic devices. However, exploring the ionizing radiation responsive APV effect remains blank, let alone its potential applications. Herein, the unprecedented APV behavior in a 1D lead‐free OIHP, (4‐AMP)BiI5 (ABI, 4‐AMP = 4‐(aminomethyl)pyridine) under X‐ray irradiation is reported, exhibiting a large above‐bandgap bulk photovoltage of ≈10 V. Such a strong APV effect is closely related to the intrinsic electric polarization in polar ABI, which acts as the driving force for X‐ray‐generated carriers' separation and transport, thus allowing it to be self‐powered. As a result, sensitive self‐powered X‐ray detectors based on high‐quality ABI single crystals are successfully fabricated, possessing a high sensitivity of 66.84 µC Gy−1 cm−2, a low detection limit of 482 nGy s−1, and superior operational stability. This work first demonstrates the ionizing radiation‐responsive APV effect in OIHPs, which further enables passive radiation detection. [ABSTRACT FROM AUTHOR]

Three‐dimensional (3D) organic–inorganic hybrid perovskites (OIHPs) have achieved tremendous success in direct X‐ray detection due to their high absorption coefficient and excellent carrier transport. However, owing to the centrosymmetry of classic 3D structures, these reported X‐ray detectors mostly require external electrical fields to run, resulting in bulky overall circuitry, high energy consumption, and operational instability. Herein, we first report the unprecedented radiation photovoltage in 3D OIHP for efficient self‐driven X‐ray detection. Specifically, the 3D polar OIHP MhyPbBr3 (1, Mhy=methylhydrazine) shows an intrinsic radiation photovoltage (0.47 V) and large mobility‐lifetime product (1.1×10−3 cm2 V−1) under X‐ray irradiation. Strikingly, these excellent physical characteristics endow 1 with sensitive self‐driven X‐ray detection performance, showing a considerable sensitivity of 220 μC Gy−1 cm−2, which surpasses those of most self‐driven X‐ray detectors. This work first explores highly sensitive self‐driven X‐ray detection in 3D polar OIHPs, shedding light on future practical applications. [ABSTRACT FROM AUTHOR]