Strategies to approach high performance in Cr3+-doped phosphors for high-power NIR-LED light sources.
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ABSTRACT:
SUBMITTER: Jia Z
PROVIDER: S-EPMC7229223 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Mn4+-activated hexafluoroaluminates are promising red-emitting phosphors for white light emitting diodes (w-LEDs). Here, we report the synthesis of Na₃AlF₆:Mn4+, K₃AlF₆:Mn4+ and K₂NaAlF₆:Mn4+ phosphors through a simple two-step co-precipitation method. Highly monodisperse large (~20 μm) smoothed-octahedron shaped crystallites are obtained for K₂NaAlF₆:Mn4+. The large size, regular shape and small size distribution are favorable for application in w-LEDs. All Mn4+-doped hexafluoroaluminates show bright red Mn4+ luminescence under blue light excitation. We compare the optical properties of Na₃AlF₆:Mn4+, K₃AlF₆:Mn4+ and K₂NaAlF₆:Mn4+ at room temperature and 4 K. The luminescence measurements reveal that multiple Mn4+ sites exist in M₃AlF₆:Mn4+ (M = Na, K), which is explained by the charge compensation that is required for Mn4+ on Al3+ sites. Thermal cycling experiments show that the site distribution changes after annealing. Finally, we investigate thermal quenching and show that the luminescence quenching temperature is high, around 460-490 K, which makes these Mn4+-doped hexafluoroaluminates interesting red phosphors for w-LEDs. The new insights reported on the synthesis and optical properties of Mn4+ in the chemically and thermally stable hexafluoroaluminates can contribute to the optimization of red-emitting Mn4+ phosphors for w-LEDs.
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Project description:Red-emitting Mn4+-doped fluorides are a promising class of materials to improve the color rendering and luminous efficacy of white light-emitting diodes (w-LEDs). For w-LEDs, the luminescence quenching temperature is very important, but surprisingly no systematic research has been conducted to understand the mechanism for thermal quenching in Mn4+-doped fluorides. Furthermore, concentration quenching of the Mn4+ luminescence can be an issue but detailed investigations are lacking. In this work, we study thermal quenching and concentration quenching in Mn4+-doped fluorides by measuring luminescence spectra and decay curves of K2TiF6:Mn4+ between 4 and 600 K and for Mn4+ concentrations from 0.01% to 15.7%. Temperature-dependent measurements on K2TiF6:Mn4+ and other Mn4+-doped phosphors show that quenching occurs through thermally activated crossover between the 4T2 excited state and 4A2 ground state. The quenching temperature can be optimized by designing host lattices in which Mn4+ has a high 4T2 state energy. Concentration-dependent studies reveal that concentration quenching effects are limited in K2TiF6:Mn4+ up to 5% Mn4+. This is important, as high Mn4+ concentrations are required for sufficient absorption of blue LED light in the parity-forbidden Mn4+ d-d transitions. At even higher Mn4+ concentrations (>10%), the quantum efficiency decreases, mostly due to direct energy transfer to quenching sites (defects and impurity ions). Optimization of the synthesis to reduce quenchers is crucial for developing more efficient highly absorbing Mn4+ phosphors. The present systematic study provides detailed insights into temperature and concentration quenching of Mn4+ emission and can be used to realize superior narrow-band red Mn4+ phosphors for w-LEDs.
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Project description:Commercial lighting for ambient and display applications is mostly based on blue light-emitting diodes (LEDs) combined with phosphor materials that convert some of the blue light into green, yellow, orange, and red. Not many phosphor materials can offer stable output under high incident light intensities for thousands of operating hours. Even the most promising LED phosphors saturate in high-power applications, that is, they show decreased light output. The saturation behavior is often poorly understood. Here, we review three popular commercial LED phosphor materials, Y3Al5O12 doped with Ce3+, CaAlSiN3 doped with Eu2+, and K2SiF6 doped with Mn4+, and unravel their saturation mechanisms. Experiments with square-wave-modulated laser excitation reveal the dynamics of absorption and decay of the luminescent centers. By modeling these dynamics and linking them to the saturation of the phosphor output intensity, we distinguish saturation by ground-state depletion, thermal quenching, and ionization of the centers. We discuss the implications of each of these processes for LED applications. Understanding the saturation mechanisms of popular LED phosphors could lead to strategies to improve their performance and efficiency or guide the development of new materials.
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