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Low‐dimensional organic–inorganic metal halides (OIMHs) have emerged as promising light emitters due to their broadband emission originating from self‐trapped excitons (STE), especially for Cu‐based OIMHs. Herein, Cu(I)‐based OIMH with a structure of (TPP)2Cu4I6·2DMSO (TPP stays for tetraphenylphosphonium, and DMSO – for dimethyl sulfoxide) has been synthesized, both in form of single crystals and as a microcrystalline powder. This compound exhibits a broadband green emission with a peak at 515 nm and a full width at half‐maximum of 78 nm, and a near‐unity photoluminescence quantum yield of 99.5%. Experimental data supported by theoretical calculations indicate that the STE emission is responsible for the green emission with a long lifetime of 2.53 µs. Down‐conversion light‐emitting device with a high luminous efficiency of 50 lm W−1 based on this compound have been fabricated, and white light has also been achieved with a high color rendering index of 96.7. Moreover, green emissive (TPP)2Cu4I6·2DMSO is utilized in scintillators for X‐ray detection and imaging, and as a luminescent ink for encryption applications. [ABSTRACT FROM AUTHOR]

Scintillators for radiation detection are of great significance in medical imaging, security, and nondestructive inspection. The current challenge for scintillators is to simultaneously achieve high scintillation light yield, fast radioluminescence, simple film fabrication, large X‐ray attenuation efficiency as well as stable and nontoxic compositions; no previous scintillators fulfill all the above requirements. Here, metal halide Rb2AgBr3, possessing defect‐bound excitonic radioluminescence, is shown as efficient and fast scintillators. This nontoxic and stable scintillator emits from excitons bound to neutral bromine vacancies, enjoying an efficient and spin‐allowed fast emission with minimized self‐absorption. Rb2AgBr3 thus has a high light yield (25 600 photons MeV−1), fast scintillation decay time (5.31 ns), and a record value of light yield versus decay time (4821 photons MeV−1 ns−1). The close‐space sublimation method is developed for fast and scalable fabrication of oriented Rb2AgBr3 films. The scintillator film is further integrated with commercial flat‐panel imagers, and the spatial resolution reaches 10.2 line pairs per millimeter at the modulation transfer function of 0.2, doubling the resolution of conventional CsI:Tl flat‐panel detectors. The dynamic X‐ray imaging and its use to real‐time monitoring of bone movement without ghosting effect is also demonstrated. [ABSTRACT FROM AUTHOR]