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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]

Environmental friendly metal halides have become emerging candidates as energy downconverting emitters for lighting and X‐ray imaging applications. Herein, luminescent single crystals of tetramethylammonium manganese chloride (C4H12NMnCl3) and tetraethylammonium bromide ((C8H20N)2MnBr4) are synthesized via a facile room‐temperature evaporation method. C4H12NMnCl3 and (C8H20N)2MnBr4 with octahedrally and tetrahedrally coordinated Mn2+ have correspondingly exhibited red and green emission peaking at 635 and 515 nm both originating from 4T1–6A1 transition of Mn2+ with high photoluminescence quantum yield (PLQY) of 91.8% and 85.1% benefiting from their specific crystal structures. Thanks to their strong photoexcitation under blue light, high PLQY, tunable emission spectra, good environmental stability, the white light‐emitting diode based on blending of C4H12NMnCl3 and (C8H20N)2MnBr4 delivers an outstanding luminous efficacy of 96 lm W−1, approaching commercial level, and shows no obvious photoluminescence intensity degradation after 3000 h under operation. In addition, manganese halides also demonstrate interesting characteristics under X‐ray excitation, C4H12NMnCl3 and (C8H20N)2MnBr4 exhibit steady‐state X‐ray light yields of 50 500 and 24 400 photons MeV−1, low detectable limits of 36.9 and 24.2 nGyair s−1, good radiation hardness, and X‐ray imaging demonstration with high‐resolution of 5 lp mm−1. This work presents a new avenue for luminescent Mn‐based metal halides toward multifunctional light‐emitting applications. [ABSTRACT FROM AUTHOR]