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Ultrafine-grained Al2O3–rare earth:yttrium aluminium garnet (Al2O3–RE:YAG) (RE = Ce; Ce+Gd) composite ceramics were obtained for the first time by reactive spark plasma sintering (SPS) using commercially available initial oxide powders. The effect of key sintering parameters (temperature, dwell time, and external pressure (Pload)) on densification peculiarities, structural-phase states, and luminescent properties of composites was studied comprehensively. Differences in phase formation and densification between Ce-doped and Ce,Gd-codoped systems were shown. Parameters of reactive SPS, at which there is partial melting with the formation of near-eutectic zones of the Al2O3–YAG system/coexistence of several variations of the YAG-type phase, were established. Pure corundum–garnet biphasic ceramics with an optimal balance between microstructural and luminescence performance were synthesized at 1425 ℃/30 min/30–60 MPa. The external quantum efficiency (EQE) of the phosphor converters reached 80.7% and 72% with close lifetime of ~63.8 ns, similar to those of commercial Ce:YAG materials, which is promising for further applications in the field of high-power white light-emitting diodes (WLEDs) and laser diodes (LDs).


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Reactive SPS of Al2O3–RE:YAG (RE = Ce; Ce+Gd) composite ceramic phosphors

Show Author's information Denis Yu. Kosyanova,b( )Anastasia A. VornovskikhaOleg O. ShichalinaEvgeniy K. PapynovaAnton A. BelovaAleksandra A. KosianovaaAleksandr N. FedoretsaAndrei A. LeonovbAlexey P. Zavjalova,cSergey A. Tikhonova,dYanbin WangeZiqiu ChengeXin Liue,fJiang Lie,f( )
Far Eastern Federal University, Vladivostok 690922, Russia
Institute of Automation and Control Processes, Far Eastern Branch of the Russian Academy of Sciences, Vladivostok 690041, Russia
Laboratory of Methods of Synchrotron Radiation, Institute of Solid State Chemistry and Mechanochemistry, Siberian Branch of the Russian Academy of Sciences, Novosibirsk 630128, Russia
Kamchatka Branch of Geophysical Survey of the Russian Academy of Sciences, Petropavlovsk-Kamchatsky 683006, Russia
Key Laboratory of Transparent Opto-functional Inorganic Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Abstract

Ultrafine-grained Al2O3–rare earth:yttrium aluminium garnet (Al2O3–RE:YAG) (RE = Ce; Ce+Gd) composite ceramics were obtained for the first time by reactive spark plasma sintering (SPS) using commercially available initial oxide powders. The effect of key sintering parameters (temperature, dwell time, and external pressure (Pload)) on densification peculiarities, structural-phase states, and luminescent properties of composites was studied comprehensively. Differences in phase formation and densification between Ce-doped and Ce,Gd-codoped systems were shown. Parameters of reactive SPS, at which there is partial melting with the formation of near-eutectic zones of the Al2O3–YAG system/coexistence of several variations of the YAG-type phase, were established. Pure corundum–garnet biphasic ceramics with an optimal balance between microstructural and luminescence performance were synthesized at 1425 ℃/30 min/30–60 MPa. The external quantum efficiency (EQE) of the phosphor converters reached 80.7% and 72% with close lifetime of ~63.8 ns, similar to those of commercial Ce:YAG materials, which is promising for further applications in the field of high-power white light-emitting diodes (WLEDs) and laser diodes (LDs).

Keywords: microstructure, luminescence performance, alumina–Ce3+-doped yttrium aluminium garnet (Al2O3–Ce:YAG) ceramic phosphors, reactive spark plasma sintering (SPS), structural-phase states

References(88)

[1]
Schubert EF, Kim JK. Solid-state light sources getting smart. Science 2005, 308: 1274–1278.
[2]
Pimputkar S, Speck JS, DenBaars SP, et al. Prospects for LED lighting. Nat Photonics 2009, 3: 180–182.
[3]
Haitz R, Tsao JY. Solid-state lighting: ‘The case’ 10 years after and future prospects. Phys Status Solidi A 2011, 208: 17–29.
[4]
Chen DQ, Xiang WD, Liang XJ, et al. Advances in transparent glass–ceramic phosphors for white light-emitting diodes— A review. J Eur Ceram Soc 2015, 35: 859–869.
[5]
Cho J, Park JH, Kim JK, et al. White light-emitting diodes: History, progress, and future. Laser Photonics Rev 2017, 11: 1600147.
[6]
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.
[7]
Ye S, Xiao F, Pan YX, et al. Phosphors in phosphor-converted white light-emitting diodes: Recent advances in materials, techniques and properties. Mater Sci Eng R 2010, 71: 1–34.
[8]
Kuritzky LY, Speck JS. Lighting for the 21st century with laser diodes based on non-basal plane orientations of GaN. MRS Commun 2015, 5: 463–473.
[9]
Wierer JJ Jr, Tsao JY, Sizov DS. Comparison between blue lasers and light-emitting diodes for future solid-state lighting. Laser Photonics Rev 2013, 7: 963–993.
[10]
Neumann A, Wierer JJ, Davis W, et al. Four-color laser white illuminant demonstrating high color-rendering quality. Opt Express 2011, 19: A982–A990.
[11]
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.
[12]
Mueller-Mach R, Mueller GO, Krames MR, et al. High-power phosphor-converted light-emitting diodes based on III-Nitrides. IEEE J Sel Top Quant 2002, 8: 339–345.
[13]
Steigerwald DA, Bhat JC, Collins D, et al. Illumination with solid state lighting technology. IEEE J Sel Top Quant 2002, 8: 310–320.
[14]
Chang MH, Das D, Varde PV, et al. Light emitting diodes reliability review. Microelectron Reliab 2012, 52: 762–782.
[15]
Tsai CC, Cheng WC, Chang JK, et al. Thermal-stability comparison of glass- and silicone-based high-power phosphor-converted white-light-emitting diodes under thermal aging. IEEE T Device Mat Re 2014, 14: 4–8.
[16]
Bachmann V, Ronda C, Meijerink A. Temperature quenching of yellow Ce3+ luminescence in YAG:Ce. Chem Mater 2009, 21: 2077–2084.
[17]
Ling JR, Zhou YF, Xu WT, et al. Red-emitting YAG:Ce,Mn transparent ceramics for warm WLEDs application. J Adv Ceram 2020, 9: 45–54.
[18]
Setlur AA. Phosphors for LED-based solid-state lighting. Electrochem Soc Interface 2009, 18: 32–36.
[19]
Mehr MY, van Driel WD, Zhang GQK. Progress in understanding color maintenance in solid-state lighting systems. Engineering 2015, 1: 170–178.
[20]
Robbins DJ. The effects of crystal field and temperature on the photoluminescence excitation efficiency of Ce3+ in YAG. J Electrochem Soc 1979, 126: 1550–1555.
[21]
Dal Lago M, Meneghini M, Trivellin N, et al. Phosphors for LED-based light sources: Thermal properties and reliability issues. Microelectron Reliab 2012, 52: 2164–2167.
[22]
Mehr MY, van Driel WD, Zhang GQ. Accelerated life time testing and optical degradation of remote phosphor plates. Microelectron Reliab 2014, 54: 1544–1548.
[23]
Zhang R, Lin H, Yu YL, et al. A new-generation color converter for high-power white LED: Transparent Ce3+:YAG phosphor-in-glass. Laser Photonics Rev 2014, 8: 158–164.
[24]
Liu SJ, He ML, Di XX, et al. CsPbX3 nanocrystals films coated on YAG:Ce3+ PiG for warm white lighting source. Chem Eng J 2017, 330: 823–830.
[25]
Yu JB, Si SC, Liu Y, et al. High-power laser-driven phosphor-in-glass for excellently high conversion efficiency white light generation for special illumination or display backlighting. J Mater Chem C 2018, 6: 8212–8218.
[26]
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.
[27]
Yao Q, Hu P, Sun P, et al. YAG:Ce3+ transparent ceramic phosphors brighten the next-generation laser-driven lighting. Adv Mater 2020, 32: 1907888.
[28]
Ratzker B, Wagner A, Kalabukhov S, et al. Controlled pore growth for enhanced photoluminescence of ceramic phosphors. Scripta Mater 2021, 202: 114008.
[29]
Cantore M, Pfaff N, Farrell RM, et al. High luminous flux from single crystal phosphor-converted laser-based white lighting system. Opt Express 2016, 24: A215–A221.
[30]
Chen DQ, Xu W, Zhou Y, et al. Color tunable dual-phase transparent glass ceramics for warm white light-emitting diodes. J Mater Chem C 2017, 5: 738–746.
[31]
Wang LL, Mei L, He G, et al. Crystallization and fluorescence properties of Ce:YAG glass–ceramics with low SiO2 content. J Lumin 2013, 136: 378–382.
[32]
Ma XG, Li XY, Li JQ, et al. Pressureless glass crystallization of transparent yttrium aluminum garnet-based nanoceramics. Nat Commun 2018, 9: 1175.
[33]
Tang YR, Zhou SM, Yi XZ, et al. Microstructure optimization of the composite phase ceramic phosphor for white LEDs with excellent luminous efficacy. Opt Lett 2015, 40: 5479–5481.
[34]
Gu C, Wang XJ, Xia C, et al. A new CaF2–YAG:Ce composite phosphor ceramic for high-power and high-color-rendering WLEDs. J Mater Chem C 2019, 7: 8569–8574.
[35]
Chen J, Weng ZX, Tang YR, et al. Fabrication of ternary ZrO2–Al2O3–YAG:Ce ceramic phosphors for white light-emitting diodes. J Eur Ceram Soc 2021, 41: 1572–1578.
[36]
Tian YN, Chen J, Yi XZ, et al. A new BaAl2O4–YAG:Ce composite ceramic phosphor for white LEDs and LDs lighting. J Eur Ceram Soc 2021, 41: 4343–4348.
[37]
Sai QL, Xia CT. Tunable colorimetric performance of Al2O3–YAG:Ce3+ eutectic crystal by Ce3+ concentration. J Lumin 2017, 186: 68–71.
[38]
Sola D, Ester FJ, Oliete PB, et al. Study of the stability of the molten zone and the stresses induced during the growth of Al2O3–Y3Al5O12 eutectic composite by the laser floating zone technique. J Eur Ceram Soc 2011, 31: 1211–1218.
[39]
Wang JC, Tang XY, Zheng P, et al. Thermally self-managing YAG:Ce–Al2O3 color converters enabling high-brightness laser-driven solid state lighting in a transmissive configuration. J Mater Chem C 2019, 7: 3901–3908.
[40]
Liu ZH, Li SX, Huang YH, et al. The effect of the porosity on the Al2O3–YAG:Ce phosphor ceramic: Microstructure, luminescent efficiency, and luminous stability in laser-driven lighting. J Alloys Compd 2019, 785: 125–130.
[41]
Zhao HY, Li Z, Zhang MW, et al. High-performance Al2O3‒YAG:Ce composite ceramic phosphors for miniaturization of high-brightness white light-emitting diodes. Ceram Int 2020, 46: 653–662.
[42]
Li SX, Zhu QQ, Tang DM, et al. Al2O3–YAG:Ce composite phosphor ceramic: A thermally robust and efficient color converter for solid state laser lighting. J Mater Chem C 2016, 4: 8648–8654.
[43]
Xu M, Chang J, Wang J, et al. Al2O3–YAG:Ce composite ceramics for high-brightness lighting. Opt Express 2019, 27: 872–885.
[44]
Kang T, Lee S, Kim J, et al. Thermal durability of YAG:Ce ceramic with containing Al2O3 and its Raman analysis. J Lumin 2020, 222: 117077.
[45]
Berman R, Foster EL, Ziman JM. Thermal conduction in artificial sapphire crystals at low temperatures I. Nearly perfect crystals. P Roy Soc A-Math Phys 1955, 231: 130–144.
[46]
Filatova EO, Konashuk AS. Interpretation of the changing the band gap of Al2O3 depending on its crystalline form: Connection with different local symmetries. J Phys Chem C 2015, 119: 20755–20761.
[47]
Cai PZ, Green DJ, Messing GL. Constrained densification of alumina/zirconia hybrid laminates, I: Experimental observations of processing defects. J Am Ceram Soc 1997, 80: 1929–1939.
[48]
Gupta TK, Valentich J. Thermal expansion of yttrium aluminum garnet. J Am Ceram Soc 1971, 54: 355–356.
[49]
Tang YR, Zhou SM, Chen C, et al. Composite phase ceramic phosphor of Al2O3–Ce:YAG for high efficiency light emitting. Opt Express 2015, 23: 17923–17928.
[50]
Liu X, Qian XL, Hu ZW, et al. Al2O3–Ce:GdYAG composite ceramic phosphors for high-power white light-emitting-diode applications. J Eur Ceram Soc 2019, 39: 2149–2154.
[51]
Ma YL, Zhang L, Zhou TY, et al. High recorded color rendering index in single Ce,(Pr,Mn):YAG transparent ceramics for high-power white LEDs/LDs. J Mater Chem C 2020, 8: 4329–4337.
[52]
Du QP, Feng SW, Qin HM, et al. Massive red-shifting of Ce3+ emission by Mg2+ and Si4+ doping of YAG:Ce transparent ceramic phosphors. J Mater Chem C 2018, 6: 12200–12205.
[53]
Hu S, Zhang YL, Wang ZJ, et al. Phase composition, microstructure and luminescent property evolutions in “light-scattering enhanced” Al2O3–Y3Al5O12:Ce3+ ceramic phosphors. J Eur Ceram Soc 2018, 38: 3268–3278.
[54]
Zhao D, Tang YR, Yi XZ, et al. High-performance Al2O3–Ce:YAG ceramics for white LED and LD by the optimization of Ce3+ concentration. Opt Mater 2020, 108: 110448.
[55]
Kosyanov DY, Liu X, Vornovskikh AA, et al. Al2O3–Ce:YAG composite ceramics for high brightness lighting: Cerium doping effect. J Alloys Compd 2021, 887: 161486.
[56]
Kosyanov DY, Yavetskiy RP, Vorona IO, et al. Transparent 4 at% Nd3+:Y3Al5O12 ceramic by reactive spark plasma sintering. AIP Conf Proc 2017, 1874: 040020.
[57]
Kosyanov DY, Vornovskikh AA, Zakharenko AM, et al. Influence of sintering parameters on transparency of reactive SPSed Nd3+:YAG ceramics. Opt Mater 2021, 112: 110760.
[58]
Kosyanov DY, Liu X, Vornovskikh AA, et al. Al2O3–Ce:YAG and Al2O3–Ce:(Y,Gd)AG composite ceramics for high brightness lighting: Effect of microstructure. Mater Charact 2021, 172: 110883.
[59]
Rodríguez-Carvajal J. Recent advances in magnetic structure determination by neutron powder diffraction. Phys B Condens Matter 1993, 192: 55–69.
[60]
[61]
Piminov PA, Baranov GN, Bogomyagkov AV, et al. Synchrotron radiation research and application at VEPP-4. Phys Procedia 2016, 84: 19–26.
[62]
Shmakov AN, Mytnichenko SV, Tsybulya SV, et al. High-resolution diffractometer for structural studies of polycrystalline materials. J Struct Chem 1994, 35: 224–228.
[63]
Wojdyr M. Fityk: A general-purpose peak fitting program. J Appl Crystallogr 2010, 43: 1126–1128.
[64]
Ancharov AI, Manakov AY, Mezentsev NA, et al. New station at the 4th beamline of the VEPP-3 storage ring. Nucl Instrum Meth A 2001, 470: 80–83.
[65]
Wurst JC, Nelson JA. Lineal intercept technique for measuring grain size in two-phase polycrystalline ceramics. J Am Ceram Soc 1972, 55: 109.
[66]
Penilla EH, Kodera Y, Garay JE. Simultaneous synthesis and densification of transparent, photoluminescent polycrystalline YAG by current activated pressure assisted densification (CAPAD). Mater Sci Eng B 2012, 177: 1178–1187.
[67]
Zavjalov AP, Shichalin OO, Tikhonov SA, et al. Features of reactive SPS of SrTiO3–TiO2 biphasic ceramics. IOP Conf Ser Mater Sci Eng 2021, 1093: 012034.
[68]
Ratzker B, Wagner A, Kalabukhov S, et al. Non-uniform microstructure evolution in transparent alumina during dwell stage of high-pressure spark plasma sintering. Acta Mater 2020, 199: 469–479.
[69]
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.
[70]
Morita K, Kim BN, Yoshida H, et al. Spark-plasma-sintering condition optimization for producing transparent MgAl2O4 spinel polycrystal. J Am Ceram Soc 2009, 92: 1208–1216.
[71]
Kosyanov DY, Baumer VN, Yavetskiy RP, et al. Nd3+:Y3Al5O12 laser ceramics: Influence of the size of yttrium oxide particles on sintering. Crystallogr Rep 2015, 60: 299–305.
[72]
Kosyanov DY, Yavetskiy RP, Kryzhanovska OS, et al. Reactive SPS of Nd3+:YAG transparent ceramics with LiF sintering additive. Opt Mater 2021, 119: 111389.
[73]
Barsoum MW. Fundamentals of Ceramics. Boca Raton, USA: CRC Press, 2002.
DOI
[74]
Marlot C. Elaboration de céramiques transparentes Er YAG: Synthèse de poudre par co-précipitation et frittage SPS. Ph.D. Thesis. Dijon, France: University of Burgundy, 2013. (in French)
[75]
Wagner A, Ratzker B, Kalabukhov S, et al. Highly-doped Nd:YAG ceramics fabricated by conventional and high pressure SPS. Ceram Int 2019, 45: 12279–12284.
[76]
Muñoz-García AB, Pascual JL, Barandiarán Z, et al. Structural effects and 4f–5d transition shifts induced by La codoping in Ce-doped yttrium aluminum garnet: First-principles study. Phys Rev B 2010, 82: 064114.
[77]
Latynina A, Watanabe M, Inomata D, et al. Properties of Czochralski grown Ce,Gd:Y3Al5O12 single crystal for white light-emitting diode. J Alloys Compd 2013, 553: 89–92.
[78]
Bernard-Granger G, Benameur N, Guizard C, et al. Influence of graphite contamination on the optical properties of transparent spinel obtained by spark plasma sintering. Scripta Mater 2009, 60: 164–167.
[79]
Jiang DT, Hulbert DM, Anselmi-Tamburini U, et al. Optically transparent polycrystalline Al2O3 produced by spark plasma sintering. J Am Ceram Soc 2008, 91: 151–154.
[80]
Bennison SJ, Harmer MP. Swelling of hot-pressed Al2O3. J Am Ceram Soc 1985, 68: 591–597.
[81]
Reimanis I, Kleebe HJ. A review on the sintering and microstructure development of transparent spinel (MgAl2O4). J Am Ceram Soc 2009, 92: 1472–1480.
[82]
Coble RL. Diffusion models for hot pressing with surface energy and pressure effects as driving forces. J Appl Phys 1970, 41: 4798–4807.
[83]
Shao C, Zhang L, Zhou TY, et al. Tunable blue/yellow emission in high-power white LED devices packaged with Ce:(Y,Gd)AG transparent ceramics. Ceram Int 2019, 45: 14420–14425.
[84]
Tan CM, Singh P, Zhao WY, et al. Physical limitations of phosphor layer thickness and concentration for white LEDs. Sci Rep 2018, 8: 2452.
[85]
Liu S, Sun P, Liu YF, et al. Warm white light with a high color-rendering index from a single Gd3Al4GaO12:Ce3+ transparent ceramic for high-power LEDs and LDs. ACS Appl Mater Interfaces 2019, 11: 2130–2139.
[86]
Sun P, Hu P, Liu YF, et al. Broadband emissions from Lu2Mg2Al2Si2O12:Ce3+ plate ceramic phosphors enable a high color-rendering index for laser-driven lighting. J Mater Chem C 2020, 8: 1405–1412.
[87]
Barzowska J, Kubicki A, Grinberg M, et al. Photoluminescence kinetics of YAG crystals activated with Ce, and Ce and Mg. Acta Phys Pol A 1999, 95: 395–402.
[88]
Leyre S, Coutino-Gonzalez E, Joos JJ, et al. Absolute determination of photoluminescence quantum efficiency using an integrating sphere setup. Rev Sci Instrum 2014, 85: 123115.
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Publication history

Received: 22 November 2022
Revised: 21 February 2023
Accepted: 24 February 2023
Published: 04 May 2023
Issue date: May 2023

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© The Author(s) 2023.

Acknowledgements

This work was supported by the Russian Science Foundation (No. 20-73-10242). Also, this work was partially supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDA22010301), the International Partnership Program of Chinese Academy of Sciences (No. 121631KYSB20200039), and the International Cooperation Project of Shanghai Science and Technology Commission (No. 20520750200). Denis Yu. Kosyanov is grateful to the Council on grants of the President of the Russian Federation (No. SP-3221.2022.1) for supporting the studies devoted to obtaining advanced ceramic materials. The SR XRD measurements were done at the shared research center SSTRC on the basis of the VEPP-4–VEPP-2000 complex at the Budker Institute of Nuclear Physics SB RAS.

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