Cation-vacancy induced intrinsic magnetism in GaN and BN is investigated by employing density-functional theory based electronic structure methods. The strong localization of defect states favors spontaneous spin polarization and local moment formation. A neutral cation vacancy in GaN or BN leads to the formation of a net moment of 3 muB with a spin-polarization energy of about 0.5 eV at the low density limit. The extended tails of defect wave functions, on the other hand, mediate surprisingly long-range magnetic interactions between the defect-induced moments. This duality of defect states suggests the existence of defect-induced or mediated collective magnetism in these otherwise nonmagnetic sp systems.
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.
All‐inorganic perovskite quantum dots (QDs) CsPbX3 (X = Cl, Br, and I) have recently emerged as a new promising class of X‐ray scintillators. However, the instability of perovskite QDs and the strong optical scattering of the thick opaque QD scintillator film imped it to realize high‐quality and robust X‐ray image. Herein, the europium (Eu) doped CsPbBr3 QDs are in situ grown inside transparent amorphous matrix to form glass‐ceramic (GC) scintillator with glass phase serving as both matrix and encapsulation for the perovskite QD scintillators. The small amount of Eu dopant optimizes the crystallization of CsPbBr3 QDs and makes their distribution more uniform in the glass matrix, which can significantly reduce the light scattering and also enhance the photoluminescence emission of CsPbBr3 QDs. As a result, a remarkably high spatial resolution of 15.0 lp mm−1 is realized thanks to the reduced light scattering, which is so far a record resolution for perovskite scintillator based X‐ray imaging, and the scintillation stability is also significantly improved compared to the bare perovskite QD scintillators. Those results provide an effective platform particularly for the emerging perovskite nanocrystal scintillators to reduce light scattering and improve radiation hardness.
Perovskite (LaSr)MnIrO (x = 0 (LSM) and 0.05 (LSMI)) nanoparticles with particle size of 20-50 nm are prepared by the polymer-assisted chemical solution method and demonstrated as high performance bifunctional oxygen catalyst in alkaline solution. As compared with LSM, LSMI with the A-site deficiency and the B-site iridium (Ir)-doping has a larger lattice, lower valence state of transition metal, and weaker metal-OH bonding; therefore, it increases the concentration of oxygen vacancy and enhances both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). LSMI exhibits superior ORR performance with only 30 mV onset potential difference from the commercial Pt/C catalyst and significant enhancement in electrocatalytic activity in the OER process, resulting in the best oxygen electrode material among all the reported perovskite oxides. LSMI also exhibits high durability for both ORR (only 18 mV negative shift for the half-wave potential compared with the initial ORR) and OER process with 10% decay. The electrochemical results indicate that the A-site deficiency and Ir-doping in perovskite oxides could be promising catalysts for the applications in fuel cells, metal-air batteries, and solar fuel synthesis.
Halide perovskites are an emerging scintillator material for X-ray imaging. High-quality X-ray imaging generally requires high spatial resolution and long operation lifetime, especially for targeted objects with irregular shapes. Herein, a perovskite "polymer-ceramics" scintillator, in which the halide perovskite nanocrystals are grown inside a pre-solidified polymer structure with high viscosity (6 × 10 12 cP), is designed to construct flexible and refreshable X-ray imaging. A nucleation inhibition strategy is proposed to prevent the agglomeration and Ostwald ripening of perovskite crystals during the subsequent precipitation process, enabling a high-quality polymer-ceramics scintillator with high transparency. This scintillator-based detector achieves a detection limit of 120 nGy s -1 and a spatial resolution of 12.5 lp mm -1 . Interestingly, due to the anchoring effect of the exfoliated atoms provided by the polymer matrix, the scintillator film can be refreshed after a long duration (≥3 h) and high dose (8 mGy s -1 ) irradiation. More importantly, this inherent characteristic overcomes the long operation lifetime issue of perovskites-based scintillators. Hence, the authors' exploration of the polymer-ceramics scintillator paves the way for the development of flexible and durable perovskite scintillators that can be produced at a low operation cost.
Core-shell structure is an obvious concept to suppress surface-related deactivations in lanthanide-doped upconversion nanoparticles (UCNPs). However, no direct observation of atomic-scale surface restoration, which can improve the upconversion photoluminescence, has been reported. Here, we use aberration-corrected high-angle annular dark field scanning transmission electron microscopy to study the surface condition of KLuF:Yb,Er bare core UCNPs. Due to the very thin and uniform thickness of the UCNPs, we observe unambiguously that the recovery from surface defects enhances upconversion photoluminescence. Furthermore, the realization of dominant green lasing emission under pulsed laser excitation confirms the high crystallinity of the UCNPs.
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