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Scintillators, which can convert high‐energy ionizing radiation (e.g., X‐ or γ‐rays) into ultraviolet‐visible light, have been widely applied in medical and industrial fields. Developing new scintillation materials with high performance and low cost is very desirable in order to address the growing application demands. Among them, single‐crystal scintillators of organic‐inorganic hybrid metal halides (OIMHs) have attracted much attention because of their excellent optical transparency, suppressed light scattering, and facile solution preparation methods. Herein, three new centimeter‐sized (2‐DMAP)2MnX4 (2‐DMAP+ = 2‐dimethylaminopyridinium, X = Cl, Br, I) single crystals with high crystal quality are synthesized via the solvent evaporation method. Benefiting from the high optical transparency and remarkable luminescence property, (2‐DMAP)2MnBr4 delivers a high X‐ray light yield of 22 000 photons MeV−1, a low limit of detection of 9.50 nGy s−1, and an excellent X‐ray imaging spatial resolution of 20–25 lp mm−1. Moreover, the regulation of single‐crystal thickness from 0.31 mm to 3.03 mm can be easily achieved via a simple solution post‐treatment method, which has a significant influence on the transmittance, spatial imaging resolution, and detection limit. This work demonstrates a promising single‐crystal scintillator for the application of high‐resolution X‐ray imaging with low preparation cost and tunable thickness. [ABSTRACT FROM AUTHOR]

Organic–inorganic hybrid copper(I)‐based halides have attracted great interest in the field of optoelectronics due to their low cost, non‐toxicity, large Stokes shift, and high photoluminescence quantum yields (PLQYs). Here, bulk zero‐dimensional (0D) organic‐inorganic hybrid copper(I)‐based (R,S‐2‐mpip)2Cu2I6 (mpip = methylpiperazinium, C5H14N22+) single crystals have been grown with equal stoichiometric ratios of R‐ and S‐2‐mpip ligands by chirality–racemization strategy for the first time. Interestingly, (R,S‐2‐mpip)2Cu2I6 single crystals exhibit strong blue–green photoluminescence (PL) located at 520 nm with large Stokes shift of about 230 nm and high PLQY of about 65.96%, which originates from self‐trapped excitons (STEs). More importantly, (R,S‐2‐mpip)2Cu2I6 single crystals also exhibit the strong radioluminescence (RL) at 520 nm, the fast X‐ray scintillation response with a light yield of about 47 000 photon MeV−1 and low detection limit of 6.48 nGyairs−1 when exposed to X‐ray irradiation condition, which is superior to that of other copper(I) iodide‐based hybrids. Based on the excellent characteristics, X‐ray imaging systems based on (R,S‐2‐mpip)2Cu2I6 single crystals exhibit the clear images of "QFNU" logo and crystal symbol pattern. This work not only deepens the understandings of material design and fundamental properties of these racemate systems, but also provides guidance for the further applications in the multi‐functional optoelectronics. [ABSTRACT FROM AUTHOR]

Low‐dimensional perovskite halides have shown a great potential as X‐ray detection materials because of efficient exciton emissions originating from strongly spatially localized charge carriers. Nonetheless, most of them have a scintillation yield far below their theoretical limits. Here, it is found that the harvesting efficiency of produced charge carriers can be significantly enhanced via a small amount of In+ doping in these highly localized structures. A bright and sensitive zero‐dimensional Cs3Cu2I5:In+ halide with efficient and tunable dual emission is reported. The radioluminescence emission of Cs3Cu2I5:In+ crystals under X‐ray excitation consists of a self‐trapped exciton emission at 460 nm and an In+‐related emission at 620 nm at room temperature. In+ doping enhances the photoluminescence quantum efficiency (PLQY) of Cs3Cu2I5 from 68.1% to 88.4%. Benefiting from the higher PLQY, Cs3Cu2I5:In+ can achieve an excellent X‐ray detection limit of 96.2 nGyair s−1, and a superior scintillation yield of 53 000 photons per MeV, which is comparable to commercial CsI:Tl single crystals. As a result, a remarkable X‐ray imaging resolution of 18 line pairs mm–1 is demonstrated, which is so far a record resolution for single crystal perovskite‐based flat‐panel detectors. These results highlight the importance of efficient harvesting of carriers (and excitons) in low‐dimensional perovskites for radiation detection applications. [ABSTRACT FROM AUTHOR]