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1.
ACS Appl Mater Interfaces ; 15(5): 7083-7101, 2023 Feb 08.
Article in English | MEDLINE | ID: mdl-36700535

ABSTRACT

Red emission from Mn4+-containing oxides inspired the development of high color rendering and cost-effective white-light-emitting diodes (WLEDs). Aiming at this fact, a series of new crystallographic site modified (Mg, Ba)3M2GeO8: Mn4+ (M = Al, Ga) compositions were developed with strong deep-red emission in the reaction to UV and blue lights. The Mg3Al2GeO8 host is composed of three phases: orthorhombic-Mg3Ga2GeO8, orthorhombic-Mg2GeO4, and cubic-MgAl2O4. However, Mg3Ga2GeO8 secured an orthorhombic crystal structure. Interestingly, Mg3Al2GeO8: Mn4+ showed a 13-fold more intense emission than Mg3Ga2GeO8: Mn4+ since Mn4+ occupancy was preferable to [AlO6] sites compared to [GaO6]. The coexisting phases of MgAl2O4 and Mg2GeO4 in Mg3Al2GeO8: Mn4+ contributed to Mn4+ luminescence by providing additional [AlO6] and [MgO6] octahedrons for Mn4+ occupancy. Further, these sites reduced the natural reduction probability of Mn4+ to Mn2+ in [AlO4] tetrahedrons, which was confirmed using cathodoluminescence analysis for the first time. A cationic substitution strategy was employed on Mg3M2GeO8: Mn4+ to improve the luminescence, and Mg3-xBaxM2GeO8: Mn4+ (M = Al, Ga) phosphors were synthesized. Partial substitution of larger Ba2+ ions in Mg2+ sites caused structural distortions and generated a new Ba impurity phase, which improved the photoluminescence. Compositionally tuned Mg2.73Ba0.27Al1.993GeO8: 0.005Mn4+ exhibited a 35-fold higher emission than that of Mg3Ga1.993GeO8: 0.005Mn4+. Additionally, this could retain 70% of its ambient emission intensity at 453 K. A warm WLED with a correlated color temperature (CCT) of 3730 K and a CRI of 89 was fabricated by combining the optimized red component with Y3Al5O12: Ce3+ and 410 nm blue LED. By tuning the ratio of blue (BaMgAl10O17: Eu2+), green (Ce0.63Tb0.37MgAl11O19), and red (Mg2.73Ba0.27Al2GeO8: 0.005Mn4+) phosphors, another WLED was developed using a 280 nm UV-LED chip. This showed natural white emission with a CRI of 79 and a CCT of 5306 K. Meanwhile, three red LEDs were also fabricated using the Mg2.73Ba0.27Al1.993GeO8: 0.005Mn4+ phosphor with commercial sources. These could be potential pc-LEDs for plant growth applications.

2.
Nanomaterials (Basel) ; 11(10)2021 Sep 29.
Article in English | MEDLINE | ID: mdl-34684990

ABSTRACT

We demonstrate flexible red light-emitting diodes based on axial GaPAs/GaP heterostructured nanowires embedded in polydimethylsiloxane membranes with transparent electrodes involving single-walled carbon nanotubes. The GaPAs/GaP axial nanowire arrays were grown by molecular beam epitaxy, encapsulated into a polydimethylsiloxane film, and then released from the growth substrate. The fabricated free-standing membrane of light-emitting diodes with contacts of single-walled carbon nanotube films has the main electroluminescence line at 670 nm. Membrane-based light-emitting diodes (LEDs) were compared with GaPAs/GaP NW array LED devices processed directly on Si growth substrate revealing similar electroluminescence properties. Demonstrated membrane-based red LEDs are opening an avenue for flexible full color inorganic devices.

3.
Nanomaterials (Basel) ; 11(6)2021 Jun 07.
Article in English | MEDLINE | ID: mdl-34200237

ABSTRACT

We propose and demonstrate both flexible and stretchable blue light-emitting diodes based on core/shell InGaN/GaN quantum well microwires embedded in polydimethylsiloxane membranes with strain-insensitive transparent electrodes involving single-walled carbon nanotubes. InGaN/GaN core-shell microwires were grown by metal-organic vapor phase epitaxy, encapsulated into a polydimethylsiloxane film, and then released from the growth substrate. The fabricated free-standing membrane of light-emitting diodes with contacts of single-walled carbon nanotube films can stand up to 20% stretching while maintaining efficient operation. Membrane-based LEDs show less than 15% degradation of electroluminescence intensity after 20 cycles of stretching thus opening an avenue for highly deformable inorganic devices.

4.
Dalton Trans ; 50(8): 3044-3059, 2021 Mar 02.
Article in English | MEDLINE | ID: mdl-33570051

ABSTRACT

The bright red emissive nature of low-cost Mn4+ ions can replace the commercially available Eu2+-doped nitrides/oxynitrides for application in white light-emitting diodes (W-LED). Herein, the Mn4+-doped Li3RbGe8O18 (LRGO) phosphor was synthesized via the solid-state reaction (SSR), microwave-assisted diffusion (MWD), and microwave-assisted sol-gel (MWS) techniques. The MWS-derived crystalline nanoparticles having sizes less than 200 nm exhibited higher red emission intensity at around 668 nm as compared to that of the micron-sized particles obtained with other approaches, owing to the improved compositional homogeneity provided by the MWS technique. The effect of microwaves was studied to gain the optimized morphology with enhanced red emission brightness. Obtained samples showed narrow red emission maxima at 668 nm under UV (300 nm) and blue (455 nm) excitations owing to 2Eg → 4A2g: Mn4+ transitions with the possibility of degeneracy. The existence of doubly degenerate forms and the splitting of 2E2g and 4A2g levels were further confirmed via low-temperature photoluminescence (PL) analysis. The emission intensity was also enhanced by the Mg2+ co-doping of MWS-derived LRGO:Mn4+ nanophosphors. Comparative photoluminescence analysis indicated that the optimized MWS route and the Mg2+ co-doping enhanced the red emission intensity by 182% as compared to the solid-state-derived LRGO:Mn4+. The optimized Mg2+ co-doped nanophosphor showed ∼99% red colour purity under UV and blue excitations. Finally, several W-LEDs were fabricated by combining the mixture of yellow-emitting YAG:Ce3+ phosphor and the optimized red-emitting LRGO:Mn4+,Mg2+ nanophosphor on a 460 nm blue-LED chip. The chromaticity of W-LEDs was tuned from bluish-white with the correlated color temperature of 6952 K, to pure white with the CCT of 5025 K. The color rendering index was also improved from 71 to 92, which could be suitable for indoor lighting applications.

5.
Nanotechnology ; 32(8): 085705, 2021 Feb 19.
Article in English | MEDLINE | ID: mdl-33171444

ABSTRACT

We analyse the electrical and optical properties of single GaN nanowire p-n junctions grown by plasma-assisted molecular-beam epitaxy using magnesium and silicon as doping sources. Different junction architectures having either a n-base or a p-base structure are compared using optical and electrical analyses. Electron-beam induced current (EBIC) microscopy of the nanowires shows that in the case of a n-base p-n junction the parasitic radial growth enhanced by the magnesium (Mg) doping leads to a mixed axial-radial behaviour with strong wire-to-wire fluctuations of the junction position and shape. By reverting the doping order p-base p-n junctions with a purely axial well-defined structure and a low wire-to-wire dispersion are achieved. The good optical quality of the top n nanowire segment grown on a p-doped stem is preserved. A hole concentration in the p-doped segment exceeding 1018 cm-3 was extracted from EBIC mapping and photoluminescence analyses. This high concentration is reached without degrading the nanowire morphology.

6.
Nanomaterials (Basel) ; 10(11)2020 Nov 16.
Article in English | MEDLINE | ID: mdl-33207755

ABSTRACT

We analyze the thermal behavior of a flexible nanowire (NW) light-emitting diode (LED) operated under different injection conditions. The LED is based on metal-organic vapor-phase deposition (MOCVD)-grown self-assembled InGaN/GaN NWs in a polydimethylsiloxane (PDMS) matrix. Despite the poor thermal conductivity of the polymer, active nitride NWs effectively dissipate heat to the substrate. Therefore, the flexible LED mounted on a copper heat sink can operate under high injection without significant overheating, while the device mounted on a plastic holder showed a 25% higher temperature for the same injected current. The efficiency of the heat dissipation by nitride NWs was further confirmed with finite-element modeling of the temperature distribution in a NW/polymer composite membrane.

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