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Ce doped Lu3Al5O12 (Ce:LuAG) transparent ceramics are considered as promising color converters for solid-state lighting because of their excellent luminous efficiency, high thermal quenching temperature, and good thermal stability. However, Ce:LuAG ceramics mainly emit green light. The shortage of red light as well as the expensive price of Lu compounds are hindering their application for white lighting. In this work, transparent (Lu,Gd)3Al5O12–Al2O3 (LuGAG–Al2O3) nanoceramics with different replacing contents of Gd3+ (10%–50%) were successfully elaborated via a glass-crystallization method. The obtained ceramics with full nanoscale grains are composed of the main LuGAG crystalline phase and secondary Al2O3 phase, exhibiting eminent transparency of 81.0%@780 nm. After doping by Ce3+, the Ce:LuGAG–Al2O3 nanoceramics show a significant red shift (510 nm→550 nm) and make up for the deficiency of red light component in the emission spectrum. The Ce:LuAG–Al2O3 nanoceramics with 20% Gd3+ show high internal quantum efficiency (81.5% in internal quantum efficiency (IQE), 96.7% of Ce:LuAG–Al2O3 nanoceramics) and good thermal stability (only 9% loss in IQE at 150 ℃). When combined with blue LED chips (10 W), 0.3%Ce:LuGAG–Al2O3 nanoceramics with 20% Gd3+ successfully realize the high-quality warm white LED lighting with a color coordinate of (0.3566, 0.435), a color temperature of 4347 K, CRI of 67.7, and a luminous efficiency of 175.8 lm·W−1. When the transparent 0.3%Ce:LuGAG–Al2O3 nanoceramics are excited by blue laser (5 W·mm2), the emission peak position redshifts from 517 to 570 nm, the emitted light exhibits a continuous change from green light to yellow light, and then to orange-yellow light, and the maximum luminous efficiency is up to 234.49 lm·W−1 (20% Gd3+). Taking into account the high quantum efficiency, good thermal stability, and excellent and adjustable luminous properties, the transparent Ce:LuGAG–Al2O3 nanoceramics with different Gd3+ substitution contents in this paper are believed to be promising candidates for high-power white LED/LD lighting.


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Biphasic (Lu,Gd)3Al5O12-based transparent nanoceramic color converters for high-power white LED/LD lighting

Show Author's information Jie Fua,b,dYing Zhangb,dShaowei Fengb,dMathieu AllixcCécile GenevoiscEmmanuel VeroncZhibiao MaaWenlong XuaLinghan BaiaRuyu FanaYafeng Yangb,dHui Wangb,dJianqiang Lia,e( )
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China
State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
CNRS, CEMHTI UPR 3079, Univ. Orléans, Orléans 45071, France
University of Chinese Academy of Sciences, Beijing 100049, China
Beijing Key Laboratory for Advanced Powder Metallurgy and Particulate Materials, University of Science and Technology Beijing, Beijing 100083, China

Abstract

Ce doped Lu3Al5O12 (Ce:LuAG) transparent ceramics are considered as promising color converters for solid-state lighting because of their excellent luminous efficiency, high thermal quenching temperature, and good thermal stability. However, Ce:LuAG ceramics mainly emit green light. The shortage of red light as well as the expensive price of Lu compounds are hindering their application for white lighting. In this work, transparent (Lu,Gd)3Al5O12–Al2O3 (LuGAG–Al2O3) nanoceramics with different replacing contents of Gd3+ (10%–50%) were successfully elaborated via a glass-crystallization method. The obtained ceramics with full nanoscale grains are composed of the main LuGAG crystalline phase and secondary Al2O3 phase, exhibiting eminent transparency of 81.0%@780 nm. After doping by Ce3+, the Ce:LuGAG–Al2O3 nanoceramics show a significant red shift (510 nm→550 nm) and make up for the deficiency of red light component in the emission spectrum. The Ce:LuAG–Al2O3 nanoceramics with 20% Gd3+ show high internal quantum efficiency (81.5% in internal quantum efficiency (IQE), 96.7% of Ce:LuAG–Al2O3 nanoceramics) and good thermal stability (only 9% loss in IQE at 150 ℃). When combined with blue LED chips (10 W), 0.3%Ce:LuGAG–Al2O3 nanoceramics with 20% Gd3+ successfully realize the high-quality warm white LED lighting with a color coordinate of (0.3566, 0.435), a color temperature of 4347 K, CRI of 67.7, and a luminous efficiency of 175.8 lm·W−1. When the transparent 0.3%Ce:LuGAG–Al2O3 nanoceramics are excited by blue laser (5 W·mm2), the emission peak position redshifts from 517 to 570 nm, the emitted light exhibits a continuous change from green light to yellow light, and then to orange-yellow light, and the maximum luminous efficiency is up to 234.49 lm·W−1 (20% Gd3+). Taking into account the high quantum efficiency, good thermal stability, and excellent and adjustable luminous properties, the transparent Ce:LuGAG–Al2O3 nanoceramics with different Gd3+ substitution contents in this paper are believed to be promising candidates for high-power white LED/LD lighting.

Keywords: glass crystallization, high-power WLEDs/LDs, white lighting, (Lu,Gd)3Al5O12 (LuGAG)–Al2O3 nanoceramics

References(51)

[1]
Feng SW, Guo YC, Allix M, et al. Biphasic Lu3MgAl3SiO12-based transparent ceramics for uniform laser-diode-driven white lighting. Cell Rep Phys Sci 2022, 3: 101044.
[2]
Pust P, Schmidt PJ, Schnick W. A revolution in lighting. Nat Mater 2015, 14: 454–458.
[3]
Schubert EF, Kim JK. Solid-state light sources getting smart. Science 2005, 308: 1274–1278.
[4]
Shur MS, Zukauskas R. Solid-state lighting: Toward superior illumination. Proc IEEE 2005, 93: 1691–1703.
[5]
Peng Y, Yu ZK, Zhao JZ, et al. Unique sandwich design of high-efficiency heat-conducting phosphor-in-glass film for high-quality laser-driven white lighting. J Adv Ceram 2022, 11: 1889–1900.
[6]
Zhou TY, Hou C, Zhang L, et al. Efficient spectral regulation in Ce:Lu3(Al,Cr)5O12 and Ce:Lu3(Al,Cr)5O12/Ce:Y3Al5O12 transparent ceramics with high color rendering index for high-power white LEDs/LDs. J Adv Ceram 2021, 10: 1107–1118.
[7]
Wu HJ, Wu H, Pan GH, et al. Cyan-green-emitting Ca3Sc2Si3O12:Ce3+ transparent ceramics: A promising color converter for high-brightness laser lighting. J Adv Ceram 2023, 12: 1731–1741.
[8]
Paucek I, Appolloni E, Pennisi G, et al. LED lighting systems for horticulture: Business growth and global distribution. Sustainability 2020, 12: 7516.
[9]
Wang YJ, Alonso JM, Ruan XB. A review of LED drivers and related technologies. IEEE T Ind Electron 2017, 64: 5754–5765.
[10]
Yazdan Mehr M, Bahrami A, van Driel WD, et al. Degradation of optical materials in solid-state lighting systems. Int Mater Rev 2020, 65: 102–128.
[11]
Zabiliūtė-Karaliūnė A, Aglinskaitė J, Vitta PK. The reduction of the thermal quenching effect in laser-excited phosphor converters using highly thermally conductive hBN particles. Sci Rep 2021, 11: 6755.
[12]
Cozzan C, Lheureux G, O'Dea N, et al. Stable, heat-conducting phosphor composites for high-power laser lighting. ACS Appl Mater Interfaces 2018, 10: 5673–5681.
[13]
Wu HJ, Pan GH, Hao ZD, et al. Highly efficient and thermally robust cyan-green phosphor-in-glass films for high-brightness laser lighting. J Mater Chem C 2021, 9: 12342–12352.
[14]
Yeh CT, Chou YN, Yang KS, et al. Luminescence material characterizations on laser-phosphor lighting techniques. Opt Express 2019, 27: 7226–7236.
[15]
Zabiliūtė-Karaliūnė A, Aglinskaitė J, Vitta PK. The reduction of the thermal quenching effect in laser-excited phosphor converters using highly thermally conductive hBN particles. Sci Rep 2021, 11: 6755.
[16]
Zhou TY, Zhang L, Shao C, et al. Sintering additives regulated Cr ion charge state in Cr doped YAG transparent ceramics. Ceram Int 2018, 44: 13820–13826.
[17]
Li Y, Hu LL, Yang BB, et al. Effect of hydrogen annealing on the photoluminescence properties of colour conversion glass in borosilicate glass. J Alloys Compd 2017, 708: 1201–1205.
[18]
Bechtel H, Schmidt PJ, Tücks A, et al. Fully phosphor-converted LEDs with Lumiramic phosphor technology. In: Proceedings of the 10th International Conference on Solid State Lighting, 2010: 7784.
DOI
[19]
Lin H, Hu T, Cheng Y, et al. Glass ceramic phosphors: Towards long-lifetime high-power white light-emitting-diode applications—A review. Laser Photonics Rev 2018, 12: 1700344.
[20]
Chung WJ, Nam YH. Review—A review on phosphor in glass as a high power LED color converter. ECS J Solid State Sc 2019, 9: 016010.
[21]
He MT, Jia JN, Zhao JJ, et al. Glass-ceramic phosphors for solid state lighting: A review. Ceram Int 2021, 47: 2963–2980.
[22]
Peng Y, Yu ZK, Zhao JZ, et al. Unique sandwich design of high-efficiency heat-conducting phosphor-in-glass film for high-quality laser-driven white lighting. J Adv Ceram 2022, 11: 1889–1900.
[23]
Balci MH, Chen F, Cunbul AB, et al. Comparative study of blue laser diode driven cerium-doped single crystal phosphors in application of high-power lighting and display technologies. Opt Rev 2018, 25: 166–174.
[24]
Xu J, Thorseth A, Xu C, et al. Investigation of laser-induced luminescence saturation in a single-crystal YAG:Ce phosphor: Towards unique architecture, high saturation threshold, and high-brightness laser-driven white lighting. J Lumin 2019, 212: 279–285.
[25]
Ma XG, Li XY, Li JQ, et al. Pressureless glass crystallization of transparent yttrium aluminum garnet-based nanoceramics. Nat Commun 2018, 9: 1175.
[26]
Yuan Y, Wang DZ, Zhou BJ, et al. High luminous fluorescence generation using Ce:YAG transparent ceramic excited by blue laser diode. Opt Mater Express 2018, 8: 2760.
[27]
Li SX, Wang L, Hirosaki N, et al. Color conversion materials for high-brightness laser-driven solid-state lighting. Laser Photonics Rev 2018, 12: 1800173.
[28]
Ma CY, Cao YG. Phosphor converters for laser driven light sources. Appl Phys Lett 2021, 118: 210503.
[29]
Wu X, Lin JF, Xu Z, et al. Defect management and multi-mode optoelectronic manipulations via photo-thermochromism in smart windows. Laser Photonics Rev 2021, 15: 2100211.
[30]
Lin JF, Zhou Y, Lu QL, et al. Reversible modulation of photoenergy in Sm-doped (K0.5Na0.5)NbO3 transparent ceramics via photochromic behavior. J Mater Chem A 2019, 7: 19374–19384.
[31]
Wang ZJ, Zhou GH, Jiang DY, et al. Recent development of A2B2O7 system transparent ceramics. J Adv Ceram 2018, 7: 289–306.
[32]
Kang J, Zhang L, Li YB, et al. Luminescence declining behaviors in YAG:Ce transparent ceramics for high power laser lighting. J Mater Chem C 2019, 7: 14357–14365.
[33]
Liu X, Zhou HY, Hu ZW, et al. Transparent Ce:GdYAG ceramic color converters for high-brightness white LEDs and LDs. Opt Mater 2019, 88: 97–102.
[34]
Sun BH, Zhang L, Zhou TY, et al. Protected-annealing regulated defects to improve optical properties and luminescence performance of Ce:YAG transparent ceramics for white LEDs. J Mater Chem C 2019, 7: 4057–4065.
[35]
Hua H, Feng SW, Ouyang ZY, et al. YAGG:Ce transparent ceramics with high luminous efficiency for solid-state lighting application. J Adv Ceram 2019, 8: 389–398.
[36]
Feng SW, Qin HM, Wu GQ, et al. Spectrum regulation of YAG:Ce transparent ceramics with Pr,Cr doping for white light emitting diodes application. J Eur Ceram Soc 2017, 37: 3403–3409.
[37]
Bachmann V, Ronda C, Meijerink A. Temperature quenching of yellow Ce3+ luminescence in YAG:Ce. Chem Mater 2009, 21: 2077–2084.
[38]
Setlur AA, Heward WJ, Gao Y, et al. Crystal chemistry and luminescence of Ce3+-doped Lu2CaMg2(Si,Ge)3O12 and its use in LED based lighting. Chem Mater 2006, 18: 3314–3322.
[39]
Li K, Shi Y, Jia FQ, et al. Low etendue yellow-green solid-state light generation by laser-pumped LuAG:Ce ceramic. IEEE Photonic Tech L 2018, 30: 939–942.
[40]
Zhang YL, Hu S, Wang ZJ, et al. Pore-existing Lu3Al5O12:Ce ceramic phosphor: An efficient green color converter for laser light source. J Lumin 2018, 197: 331–334.
[41]
Xu J, Wang J, Gong YX, et al. Investigation of an LuAG: Ce translucent ceramic synthesized via spark plasma sintering: Towards a facile synthetic route, robust thermal performance, and high-power solid state laser lighting. J Eur Ceram Soc 2018, 38: 343–347.
[42]
Chen L, Lin CC, Yeh CW, et al. Light converting inorganic phosphors for white light-emitting diodes. Materials, 3: 2172–2195.
[43]
Wang HM, Lu ZW, Huang ZY, et al. Size effect on hardness for micro-sized and nano-sized YAG transparent ceramics. Ceram Int 2018, 44: 12472–12476.
[44]
Chen XQ, Qin HM, Zhang Y, et al. Fabrication of cerium-doped nonstoichiometric (Ce,Lu,Gd)3+δ(Ga,Al)5–δO12 transparent ceramics. J Rare Earth 2015, 33: 863–866.
[45]
Qian XL, Shi MM, Yang BB, et al. Thermostability and reliability properties studies of transparent Ce:GdYAG ceramic by Gd substitution for white LEDs. Opt Mater 2019, 94: 172–181.
[46]
Fu J, Feng SW, Guo YC, et al. Ce3+:Lu3Al5O12–Al2O3 optical nanoceramic scintillators elaborated via a low-temperature glass crystallization route. J Adv Ceram 2023, 12: 268–278.
[47]
Li JK, Li JG, Liu SH, et al. The development of Ce3+-activated (Gd,Lu)3Al5O12 garnet solid solutions as efficient yellow-emitting phosphors. Sci Technol Adv Mat 2013, 14: 054201.
[48]
Meng QH, Zhu Q, Li XD, et al. New Mg2+/Ge4+-stabilized Gd3MgxGexAl5−2xO12:Ce garnet phosphor with orange-yellow emission for warm-white LEDs (x = 2.0–2.5). Inorg Chem 2021, 60: 9773–9784.
[49]
Zheng P, Li SX, Takeda T, et al. Unraveling the luminescence quenching of phosphors under high-power-density excitation. Acta Mater 2021, 209: 116813.
[50]
Yu ZK, Zhao JZ, Wang Q, et al. Laser spot associated high-saturation phosphor-in-glass film for transmissive and reflective high-brightness laser lighting. J Adv Ceram 2023, 12: 1821–1832.
[51]
Cheng ZQ, Liu X, Chen XR, et al. Composition and luminescence properties of highly robust green-emitting LuAG:Ce/Al2O3 composite phosphor ceramics for high-power solid-state lighting. J Adv Ceram 2023, 12: 625–633.
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Publication history

Received: 30 August 2023
Revised: 08 October 2023
Accepted: 26 October 2023
Published: 04 January 2024
Issue date: December 2023

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© The Author(s) 2023.

Acknowledgements

This work is financially supported by the National Natural Science Foundation of China (No. 51972304), Beijing Municipal Science & Technology Commission, Administrative Commission of Zhongguancun Science Park (No. Z221100006722022), the Project of Scientific Experiment on Chinese Manned Space Station, Chinese Academy of Sciences President’s International Fellowship Initiative for 2021 (No. 2021VEA0012), and the Fundamental Research Funds for the Central Universities. The project benefitted from the microscopy facilities of the Platform MACLE-CVL which was co-funded by the European Union and Centre-Val de Loire Region (FEDER).

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