Weak X-Ray to Visible Lights Detection Enabled by a 2D Multilayered Lead Iodide Perovskite with Iodine-Substituted Spacer.

Broadband photodetectors (PDs) with low detection limits hold significant importance to next-generation optoelectronic devices. However, simultaneously detecting broadband (i.e., X-ray to visible regimes) and weak lights in a single semiconducting material remains highly challenging. Here, by alloying iodine-substituted short-chain cations into the 3D FAPbI 3 (FA = formamidine), a new 2D bilayered lead iodide hybrid perovskite, (2IPA) 2 FAPb 2 I 7 (1, 2IPA = 2-iodopropylammonium), that enables addressing this challenge is reported. Such a 2D multilayered structure and lead iodide composition jointly endow 1 with a minimized dark current (6.04 pA), excellent electrical property, and narrow bandgap (2.03 eV), which further gives it great potential for detecting broadband weak lights. Consequently, its high-quality single crystal PDs exhibit remarkable photoresponses to weak ultraviolet-visible lights (377-637 nm) at several tens of nW cm -2 with high responsivities (>10 2  mA W -1 ) and significant detectivities (>10 12 Jones). Moreover, 1 has an excellent X-ray detection performance with a high sensitivity of 438 µC Gy -1 cm -2 and an ultralow detection limit of 20 nGy s -1 . These exceptional attributes make 1 a promising material for broadband weak lights detection, which also sheds light on future explorations of high-performance PDs based on 2D hybrid perovskites.