| Summary: | We have fabricated a photodetector based on (CH<sub>3</sub>NH<sub>3</sub>)<sub>3</sub>Sb<sub>2</sub>Br<sub>9</sub> (MA<sub>3</sub>Sb<sub>2</sub>Br<sub>9</sub>) lead-free perovskite-like single crystal, which plays an important role in the optoelectronic characteristics of the photodetector as a perovskite-like photosensitive layer. Here, MA<sub>3</sub>Sb<sub>2</sub>Br<sub>9</sub> single crystals were synthesized by an inverse temperature crystallization process with a precursor solution at three different growth temperatures, 60 °C, 80 °C, and 100 °C. As a result, a MA<sub>3</sub>Sb<sub>2</sub>Br<sub>9</sub> single crystal with an optimum growth temperature of 60 °C presented a low trap density of 2.63 × 10<sup>11</sup> cm<sup>−3</sup>, a high charge carrier mobility of 0.75 cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup>, and excellent crystal structure and optical absorption properties. This MA<sub>3</sub>Sb<sub>2</sub>Br<sub>9</sub> perovskite-like photodetector displayed a low dark current of 8.09 × 10<sup>−9</sup> A, high responsivity of 0.113 A W<sup>−1</sup>, and high detectivity of 4.32 × 10<sup>11</sup> Jones.
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