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All‐inorganic Cu‐based perovskite CsxCuyIx+y thin films are deposited with vacuum thermal evaporation using CuI and CsI mixed powder with different proportion as evaporation sources. With CuI film as buffer‐layer, the as grown CsxCuyIx+y perovskite films only have CsCu2I3 phase owing to the epitaxy on CuI layer. And the thin film quality and optoelectronic properties of CsCu2I3 are also improved. Then, metal–semiconductor–metal UV detectors based on CsCu2I3 films with Au interdigital electrodes are fabricated and the enhancement of photoresponse performance is investigated in detail. The peak responsivity and specific detectivity of the detector are 49.22 mA W−1 and 2.49 × 1012 cm Hz1/2 W−1, which are 74 and 138 times larger than that of the device without the CuI buffer‐layer, respectively.

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