Phosphor-converted white light-emitting diodes (pc-WLEDs) are efficient light sources used in lighting, high-tech displays, and electronic devices. One of the most significant challenges of pc-WLEDs is the thermal quenching, in which the phosphor suffers from emission loss with increasing temperature during high-power LED operation. Here, we report a blue-emitting NaSc(PO):xEu phosphor (λ = 453 nm) that does not exhibit thermal quenching even up to 200 °C. This phenomenon of zero thermal quenching originates from the ability of the phosphor to compensate the emission losses and therefore sustain the luminescence with increasing temperature. The findings are explained by polymorphic modification and possible energy transfer from electron-hole pairs at the thermally activated defect levels to the Eu 5d-band with increasing temperature. Our results could initiate the exploration of phosphors with zero thermal quenching for high-power LED applications.
Organolead halide perovskites have emerged as a promising optoelectronic material for lighting due to its high quantum yield, color-tunable, and narrow emission. Despite their unique properties, toxicity has intensified the search for ecofriendly alternatives through partial or complete replacement of lead. Herein, we report a roomtemperature synthesized Mn 2+ -substituted 3D-organolead perovskite displacing ∼90% of lead, simultaneously retaining its unique excitonic emission, with an additional orange emission of Mn 2+ via energy transfer. A high Mn solubility limit of 90% was attained for the first time in lead halide perovskites, facilitated by the flexible organic cation (CH 3 NH 3 ) + network, preserving the perovskite structure. The emission intensities of the exciton and Mn were influenced by the halide identity that regulates the energy transfer to Mn. Homogeneous emission and electron spin resonance characteristics of Mn 2+ indicate a uniform distribution of Mn. These results suggest that low-toxicity 3D-CH 3 NH 3 Pb 1−x Mn x Br 3−(2x+1) Cl 2x+1 nanocrystals may be exploited as magnetically doped quantum dots with unique optoelectronic properties.
A moisture-stable, red-emitting fluoride phosphor with an organic hydrophobic skin is reported. A simple strategy was employed to form a metal-free, organic, passivating skin using oleic acid (OA) as a hydrophobic encapsulant via solvothermal treatment. Unlike other phosphor coatings that suffer from initial efficiency loss, the OA-passivated KSiF:Mn (KSF-OA) phosphor exhibited the unique property of stable emission efficiency. Control of thickness and a highly transparent passivating layer helped to retain the emission efficiency of the material after encapsulation. A moisture-stable KSF-OA phosphor could be synthesized because of the exceptionally hydrophobic nature of OA and the formation of hydrogen bonds (F···H) resulting from the strong interactions between the fluorine in KSF and hydrogen in OA. The KSF-OA phosphor exhibited excellent moisture stability and maintained 85% of its emission intensity even after 450 h at high temperature (85 °C) and humidity (85%). As a proof-of-concept, this strategy was used for another moisture-sensitive SrSiON:Eu phosphor which showed enhanced moisture stability, retaining 85% of emission intensity after 500 h under the same conditions. White light-emitting devices were fabricated using surface-passivated KSF and YAlO:Ce which exhibited excellent color rendering index of 86, under blue LED excitation.
Zero-dimensional (0D) inorganic perovskites have recently emerged as an interesting class of material owing to their intrinsic Pb2+ emission, polaron formation, and large exciton binding energy. They have a unique quantum-confined structure, originating from the complete isolation of octahedra exhibiting single-molecule behavior. Herein, we probe the optical behavior of single-molecule-like isolated octahedra in 0D Cesium lead halide (Cs4PbX6, X = Cl, Br/Cl, Br) nanocrystals through isovalent manganese doping at lead sites. The incorporation of manganese induced phase stabilization of 0D Cs4PbX6 over CsPbX3 by lowering the symmetry of PbX6 via enhanced octahedral distortion. This approach enables the synthesis of CsPbX3 free Cs4PbX6 nanocrystals. A high photoluminescence quantum yield for manganese emission was obtained in colloidal (29%) and solid (21%, powder) forms. These performances can be attributed to structure-induced confinement effects, which enhance the energy transfer from localized host exciton states to Mn2+ dopant within the isolated octahedra.
Li-rich layered oxides are the most attractive cathodes for lithium-ion batteries due to their high capacity (>250 mAh g(-1)). However, their application in electric vehicles is hampered by low power density and poor cycle life. To address these, layered Li2Ru0.75Ti0.25O3 (LRTO) was synthesized and the influence of electroinactive Ti(4+) on the electrochemical performance of Li2RuO3 was investigated. LRTO exhibited a reversible capacity of 240 mAh g(-1) under 14.3 mA g(-1) with 0.11 mol of Li loss after 100 cycles compared to 0.22 mol of Li for Li2Ru0.75Sn0.25O3. More Li(+) can be extracted from LRTO (0.96 mol of Li) even after 250 cycles at 143 mA g(-1) than Li2RuO3 (0.79 mol of Li). High reversible Li extraction and long cycle life were attributed to structural stability of the LiM2 layer in the presence of Ti(4+), facilitating the lithium diffusion kinetics. The versatility of the Li2MO3 structure may initiate exploration of Ti-based Li-rich layered oxides for vehicular applications.
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