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Journal of Advanced Ceramics 2024, 13(1): 113-123 https://doi.org/10.26599/JAC.2024.9220845
Research Article | Open Access | Issue | Published: 29 January 2024

Optical grade (Gd0.95-xLuxEu0.05)3Al5O12 ceramics with near-zero optical loss: Effects of Lu3+ doping on structural feature, microstructure evolution, and far-red luminescence

Show Author's Information Zhigang Sun1,  Ji-Guang Li2,  Huiyu Qian1,  Yoshio Sakka2,  Tohru S. Suzuki2,  Bin Lu1,3( )
School of Materials Science and Chemical Engineering, Ningbo University, Ningbo 315211, China
Research Center for Electronic and Optical Materials, National Institute for Materials Science, Ibaraki 305-0044, Japan
Key Laboratory of Photoelectric Detection Materials and Devices of Zhejiang Province, Ningbo 315211, China
Keywords:
optical properties, transparent ceramics, light-emitting diode (LED), Gibbs free energy, phosphors, garnet
Cite this article:
Sun Z, Li J-G, Qian H, et al. Optical grade (Gd0.95-xLuxEu0.05)3Al5O12 ceramics with near-zero optical loss: Effects of Lu3+ doping on structural feature, microstructure evolution, and far-red luminescence. Journal of Advanced Ceramics, 2024, 13(1): 113-123. https://doi.org/10.26599/JAC.2024.9220845
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Abstract Full text Electronic supplementary material About this article

A chemical co-precipitation strategy was employed to synthesize a series of (Gd0.95−xLuxEu0.05)3Al5O12 (x = 0.1−0.95) powder phosphors, followed by vacuum sintering to achieve transparent garnet ceramic phosphors. The density functional theory indicated Lu3Al5O12 was formed in priority compared with Gd3Al5O12 during solid-phase reaction. Upon high-temperature sintering, the Lu3+ substitution for Gd3+ suppressed point mass diffusion leading to a smaller grain size. The in-line transmittances of bulk specimens with x = 0.1, 0.3, 0.5, 0.7, and 0.95 nm were ~83.5%, 80.1%, 68.8%, 73.7%, and 82.2% at 710 nm (Eu3+ emission center), respectively, among which the sample of x = 0.1 exhibited the optical grade with near-zero optical loss in agreement with the defect-free single crystal (~100% of the theoretical transmittance). The resulting particle and ceramic materials both presented characteristic Eu3+ emission arising from 5D0→7FJ (J = 1−4) transition, where the dominant far-red emission at ~710 nm arising from 5D0→7F4 transition overlapped with the absorption of phytochrome (PFR). The photoluminescence excitation and photoluminescence intensities of (Gd0.95−xLuxEu0.05)3Al5O12 powders and ceramics generally increased at a higher Gd3+/Lu3+ ratio. Lu3+ dopants delayed the fluorescence lifetime while the bulk samples had shorter lifetime compared to the particle counterparts. The transparent (Gd0.85Lu0.1Eu0.05)3Al5O12 ceramic phosphor exhibited good thermal stability with a high thermal quenching temperature above 533 K. The designed ceramic phosphor-converted light-emitting diode had a saturation injection current of 435 mA and a current-dependent color rendering index. More importantly, our report marked the developmental stage of transparent ceramic materials towards zero optical loss.


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Electronic supplementary material
About this article

Optical grade (Gd0.95-xLuxEu0.05)3Al5O12 ceramics with near-zero optical loss: Effects of Lu3+ doping on structural feature, microstructure evolution, and far-red luminescence

Show Author's information Zhigang Sun1, Ji-Guang Li2, Huiyu Qian1, Yoshio Sakka2, Tohru S. Suzuki2, Bin Lu1,3( )
School of Materials Science and Chemical Engineering, Ningbo University, Ningbo 315211, China
Research Center for Electronic and Optical Materials, National Institute for Materials Science, Ibaraki 305-0044, Japan
Key Laboratory of Photoelectric Detection Materials and Devices of Zhejiang Province, Ningbo 315211, China

Abstract

A chemical co-precipitation strategy was employed to synthesize a series of (Gd0.95−xLuxEu0.05)3Al5O12 (x = 0.1−0.95) powder phosphors, followed by vacuum sintering to achieve transparent garnet ceramic phosphors. The density functional theory indicated Lu3Al5O12 was formed in priority compared with Gd3Al5O12 during solid-phase reaction. Upon high-temperature sintering, the Lu3+ substitution for Gd3+ suppressed point mass diffusion leading to a smaller grain size. The in-line transmittances of bulk specimens with x = 0.1, 0.3, 0.5, 0.7, and 0.95 nm were ~83.5%, 80.1%, 68.8%, 73.7%, and 82.2% at 710 nm (Eu3+ emission center), respectively, among which the sample of x = 0.1 exhibited the optical grade with near-zero optical loss in agreement with the defect-free single crystal (~100% of the theoretical transmittance). The resulting particle and ceramic materials both presented characteristic Eu3+ emission arising from 5D0→7FJ (J = 1−4) transition, where the dominant far-red emission at ~710 nm arising from 5D0→7F4 transition overlapped with the absorption of phytochrome (PFR). The photoluminescence excitation and photoluminescence intensities of (Gd0.95−xLuxEu0.05)3Al5O12 powders and ceramics generally increased at a higher Gd3+/Lu3+ ratio. Lu3+ dopants delayed the fluorescence lifetime while the bulk samples had shorter lifetime compared to the particle counterparts. The transparent (Gd0.85Lu0.1Eu0.05)3Al5O12 ceramic phosphor exhibited good thermal stability with a high thermal quenching temperature above 533 K. The designed ceramic phosphor-converted light-emitting diode had a saturation injection current of 435 mA and a current-dependent color rendering index. More importantly, our report marked the developmental stage of transparent ceramic materials towards zero optical loss.

Keywords: optical properties, transparent ceramics, light-emitting diode (LED), Gibbs free energy, phosphors, garnet

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Publication history

Received: 14 October 2023
Revised: 28 November 2023
Accepted: 22 December 2023
Published: 29 January 2024
Issue date: January 2024

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© The Author(s) 2024.

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The research was supported by Zhejiang Provincial Natural Science Foundation of China (Grant No. LY23F050007).

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This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, http://creativecommons.org/licenses/by/4.0/).

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