X-rays are widely used in probing inside information nondestructively, enabling broad applications in the medical radiography and electronic industries. X-ray imaging based on emerging lead halide perovskite scintillators has received extensive attention recently. However, the strong self-absorption, relatively low light yield and lead toxicity of these perovskites restrict their practical applications. Here, we report a series of nontoxic double-perovskite scintillators of Cs 2 Ag 0.6 Na 0.4 In 1-y Bi y Cl 6. By controlling the content of the heavy atom Bi 3+ , the X-ray absorption coefficient, radiative emission efficiency, light yield and light decay were manipulated to maximise the scintillator performance. A light yield of up to 39,000 ± 7000 photons/MeV for Cs 2 Ag 0.6 Na 0.4 In 0.85 Bi 0.15 Cl 6 was obtained, which is much higher than that for the previously reported lead halide perovskite colloidal CsPbBr 3 (21,000 photons/MeV). The large Stokes shift between the radioluminescence (RL) and absorption spectra benefiting from self-trapped excitons (STEs) led to a negligible selfabsorption effect. Given the high light output and fast light decay of this scintillator, static X-ray imaging was attained under an extremely low dose of ∼1 μGy air , and dynamic X-ray imaging of finger bending without a ghosting effect was demonstrated under a low-dose rate of 47.2 μGy air s −1. After thermal treatment at 85°C for 50 h followed by X-ray irradiation for 50 h in ambient air, the scintillator performance in terms of the RL intensity and X-ray image quality remained almost unchanged. Our results shed light on exploring highly competitive scintillators beyond the scope of lead halide perovskites, not only for avoiding toxicity but also for better performance.
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 (C 4 H 12 NMnCl 3 ) and tetraethylammonium bromide ((C 8 H 20 N) 2 MnBr 4 ) are synthesized via a facile room-temperature evaporation method. C 4 H 12 NMnCl 3 and (C 8 H 20 N) 2 MnBr 4 with octahedrally and tetrahedrally coordinated Mn 2+ have correspondingly exhibited red and green emission peaking at 635 and 515 nm both originating from 4 T 1 -6 A 1 transition of Mn 2+ 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 C 4 H 12 NMnCl 3 and (C 8 H 20 N) 2 MnBr 4 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, C 4 H 12 NMnCl 3 and (C 8 H 20 N) 2 MnBr 4 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 nGy air 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.
Compact near‐infrared (NIR) light sources with broad emission band are essential to enable NIR spectroscopy compatible with portable devices, and phosphor‐converted light emitting diodes (pc‐LEDs) are efficient, low‐cost, and compact light sources. However, it is more challenging to develop highly efficient and thermally stable broadband NIR phosphors than conventional phosphors for white LEDs. Here, a series of solid solution phosphors with broadband NIR emission designed by cationic substitution in Cr3+ activated garnet Gd3Sc2Ga3O12 are reported. The internal quantum efficiency of Cr3+ emission can be significantly improved to nearly 100% via the substitution of ScO6 with smaller AlO6 octahedrons, which is attributed to the reduction of antisite defects. Moreover, the phosphor with optimized composition shows highly thermally stable emission, which renders the as‐fabricated pc‐LED with high‐power (750.8 mW) NIR emission covering the wavelength range of 700–1000 nm. The results could advance the development of NIR pc‐LEDs as high‐performance light sources for miniature NIR spectrometers.
The development of high-power white light-emitting diodes demands highly efficient and stable all-inorganic color converters. In this respect, phosphor-glass/ceramic composites show great promise as they could combine the merits of high quantum efficiency of phosphors and high chemical and thermal stabilities of glass/ceramic matrices. However, strong interfacial reaction between phosphors and matrices at high temperature results in quantum efficiency loss of the embedded phosphors, and traditional solutions rely on high-pressure consolidation techniques. Here we report the intrinsic inhibition of interfacial reaction by using silica glass rather than multicomponent glasses as the matrix. The embedment of phosphors is achieved via a pressureless sintering method, rendering these color-tunable phosphor-glass composites not only accessible to three-dimensional printing technique, but also highly efficient (internal quantum efficiency >90.0%), thermally stable at 1200 °C and hydrothermally stable at 200 °C. Our results provide a facile and general strategy for developing all-inorganic functional composites.
Phosphor‐converted light‐emitting diodes (pc‐LEDs) with broadband near‐infrared (NIR) emission have emerged as compact light sources for portable NIR spectroscopy. However, the associated broadband NIR phosphors suffer from low quantum efficiency (QE) and severe thermal quenching. Here the realization of highly efficient (internal QE ≈ 90%) and nearly zero‐thermal‐quenching broad NIR emission in Cr3+ and Yb3+ codoped Gd3Sc1.5Al0.5Ga3O12 (GSGG) via efficient energy transfer from Cr3+ to Yb3+ is reported, whereby a high‐performance NIR pc‐LED is obtained that can generate ultra‐broad‐band NIR emission covering the whole range of 700−1100 nm with high output power (50 mW at a current of 100 mA) and high photoelectric efficiency (24% at a current of 10 mA). The results not only demonstrate that Cr3+ and Yb3+ codoped GSGG has great potential for compact NIR light sources, but also indicate that the strategy of energy transfer can be exploited for developing new NIR phosphors with both high QE and thermal stability.
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