Boosting Photovoltaic Respond Through Molecular Engineering in Organic Manganese (II) Bromide for High‐Sensitivity X‑Ray Detection

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Zero‐dimensinoal (0D) manganese‐based metal halides (MHs) demonstrate excellent structural tunable through organic cation design, enabling precise control of Mn─Mn distances to modulate critical photoelectric physical properties. Here, two novel 0D PTA 2 MnBr 4 (PTA = phenyltrimethylammonium) are synthesized and DMA 2 MnBr 4 (DMA = dimethylammonium) wafer with a manipulation of octahedra are synthesized by a precise molecular design. Structural analysis reveals that the PTA‐functional group with extended π ‐conjugation lengths increases the Mn─Mn distance, results in a lower energy transfer and reduced exciton binding energy compared to DMA⁺ (linear carbon chain). Consequently, PTA 2 MnBr 4 demonstrates an enhanced photoluminescence quantum yield and prolonged exciton lifetime. The engineered X‐ray detector based on PTA 2 MnBr 4 wafer exhibits a higher sensitivity of 1122 µC Gy air −1 cm −2 and a lower detection limit of 95 nGy air s −1 , while DMA 2 MnBr 4 device are 708.2 µC Gy air −1 cm −2 and 180 nGy air s −1 , respectively, which paves the way for high‐efficiency photoelectronic applications. This suggests that molecular engineering is a robust approach for designing high‐performance 0D manganese halides for radiation detection.