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2D Dion−Jacobson (DJ) perovskite single crystals (PSCs) usually demonstrate better X‐ray detection performance than Ruddlesden‐Popper (RP) PSCs. However, the mechanism of the improved performance is still elusive. Here, by the aid of strong interactions between dimethylbiguanide (DGA) and PbI2, a novel DJ‐perovskitoid (DGA)PbI4 is designed. From the comparison of (DGA)PbI4 to other 2D PSCs, it is...
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