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Transparent Ce:lutetium aluminum garnet (Ce:Lu3Al5O12, Ce:LuAG) ceramics have been regarded as potential scintillator materials due to their relatively high density and atomic number (Zeff). However, the current Ce:LuAG ceramics exhibit a light yield much lower than the expected theoretical value due to the inevitable presence of LuAl antisite defects at high sintering temperatures. This work demonstrates a low-temperature (1100 ℃) synthetic strategy for elaborating transparent LuAG–Al2O3 nanoceramics through the crystallization of 72 mol% Al2O3–28 mol% Lu2O3 (ALu28) bulk glass. The biphasic nanostructure composed of LuAG and Al2O3 nanocrystals makes up the whole ceramic materials. Most of Al2O3 is distributed among LuAG grains, and the rest is present inside the LuAG grains. Fully dense biphasic LuAG–Al2O3 nanoceramics are highly transparent from the visible region to mid-infrared (MIR) region, and particularly the transmittance reaches 82% at 780 nm. Moreover, LuAl antisite defect-related centers are completely undetectable in X-ray excited luminescence (XEL) spectra of Ce:LuAG–Al2O3 nanoceramics with 0.3–1.0 at% Ce. The light yield of 0.3 at% Ce:LuAG–Al2O3 nanoceramics is estimated to be 20,000 ph/MeV with short 1 μs shaping time, which is far superior to that of commercial Bi4Ge3O12 (BGO) single crystals. These results show that a low-temperature glass crystallization route provides an alternative approach for eliminating the antisite defects in LuAG-based ceramics, and is promising to produce garnet-based ceramic materials with excellent properties, thereby meeting the demands of advanced scintillation applications.


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Ce3+:Lu3Al5O12–Al2O3 optical nanoceramic scintillators elaborated via a low-temperature glass crystallization route

Show Author's information Jie Fua,b,dShaowei Fengb,dYongchang Guob,dYing Zhangb,dCécile GenevoiscEmmanuel VeroncMathieu Allixc( )Jianqiang Lia( )
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China
State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
CNRS, CEMHTI UPR 3079, Université d’Orléans, Orléans 45071, France
University of Chinese Academy of Sciences, Beijing 100049, China

Abstract

Transparent Ce:lutetium aluminum garnet (Ce:Lu3Al5O12, Ce:LuAG) ceramics have been regarded as potential scintillator materials due to their relatively high density and atomic number (Zeff). However, the current Ce:LuAG ceramics exhibit a light yield much lower than the expected theoretical value due to the inevitable presence of LuAl antisite defects at high sintering temperatures. This work demonstrates a low-temperature (1100 ℃) synthetic strategy for elaborating transparent LuAG–Al2O3 nanoceramics through the crystallization of 72 mol% Al2O3–28 mol% Lu2O3 (ALu28) bulk glass. The biphasic nanostructure composed of LuAG and Al2O3 nanocrystals makes up the whole ceramic materials. Most of Al2O3 is distributed among LuAG grains, and the rest is present inside the LuAG grains. Fully dense biphasic LuAG–Al2O3 nanoceramics are highly transparent from the visible region to mid-infrared (MIR) region, and particularly the transmittance reaches 82% at 780 nm. Moreover, LuAl antisite defect-related centers are completely undetectable in X-ray excited luminescence (XEL) spectra of Ce:LuAG–Al2O3 nanoceramics with 0.3–1.0 at% Ce. The light yield of 0.3 at% Ce:LuAG–Al2O3 nanoceramics is estimated to be 20,000 ph/MeV with short 1 μs shaping time, which is far superior to that of commercial Bi4Ge3O12 (BGO) single crystals. These results show that a low-temperature glass crystallization route provides an alternative approach for eliminating the antisite defects in LuAG-based ceramics, and is promising to produce garnet-based ceramic materials with excellent properties, thereby meeting the demands of advanced scintillation applications.

Keywords: nanoceramics, glass crystallization, garnet antisite defects, Lu3Al5O12–Al2O3 (LuAG–Al2O3) transparent ceramics, scintillation

References(51)

[1]
Nikl M, Yoshikawa A. Recent R&D trends in inorganic single-crystal scintillator materials for radiation detection. Adv Opt Mater 2015, 3: 463–481.
[2]
Xu X, Lebbou K, Moretti F, et al. Ce-doped LuAG single-crystal fibers grown from the melt for high-energy physics. Acta Mater 2014, 67: 232–238.
[3]
Hu ZW, Cao MQ, Chen HH, et al. The role of air annealing on the optical and scintillation properties of Mg co-doped Pr:LuAG transparent ceramics. Opt Mater 2017, 72: 201–207.
[4]
Nikl M, Yoshikawa A, Kamada K, et al. Development of LuAG-based scintillator crystals—A review. Prog Cryst Growth Ch 2013, 59: 47–72.
[5]
Chewpraditkul W, Sreebunpeng K, Nikl M, et al. Comparison of Lu3Al5O12:Pr3+ and Bi4Ge3O12 scintillators for gamma-ray detection. Radiat Meas 2012, 47: 1–5.
[6]
Chen XP, Hu ZW, Dai JW, et al. The influence of air annealing on the microstructure and scintillation properties of Ce,Mg:LuAG ceramics. J Am Ceram Soc 2019, 102: 1805–1813.
[7]
Ma WQ, Jiang BX, Feng XQ, et al. On fast LuAG:Ce scintillation ceramics with Ca2+ co-dopants. J Am Ceram Soc 2021, 104: 966–973.
[8]
Ikesue A, Aung YL. Ceramic laser materials. Nat Photonics 2008, 2: 721–727.
[9]
Messing GL, Stevenson AJ. Toward pore-free ceramics. Science 2008, 322: 383–384.
[10]
Hinklin TR, Rand SC, Laine RM. Transparent, polycrystalline upconverting nanoceramics: Towards 3-D displays. Adv Mater 2008, 20: 1270–1273.
[11]
Van Eijk CW. Inorganic scintillators in medical imaging. Phys Med Biol 2002, 47: R85–R106.
[12]
Gerasymov I, Nepokupnaya T, Boyarintsev A, et al. GAGG:Ce composite scintillator for X-ray imaging. Opt Mater 2020, 109: 110305.
[13]
Yanagida T, Fujimoto Y, Yokota Y, et al. Comparative study of transparent ceramic and single crystal Ce doped LuAG scintillators. Radiat Meas 2011, 46: 1503–1505.
[14]
Yanagida T, Fujimoto Y, Kamada K, et al. Scintillation properties of transparent ceramic Pr:LuAG for different Pr concentration. IEEE Trans Nucl Sci 2012, 59: 2146– 2151.
[15]
Hu C, Feng XQ, Li J, et al. Role of Y admixture in (Lu1−xYx)3Al5O12:Pr ceramic scintillators free of host luminescence. Phys Rev Appl 2016, 6: 064026.
[16]
Wu YT, Luo ZH, Jiang HC, et al. Single crystal and optical ceramic multicomponent garnet scintillators: A comparative study. Nucl Instrum Meth A 2015, 780: 45–50.
[17]
Dorenbos P. Fundamental limitations in the performance of Ce3+-, Pr3+-, and Eu2+-activated scintillators. IEEE Trans Nucl Sci 2010, 57: 1162–1167.
[18]
Nikl M, Mihokova E, Pejchal J, et al. The antisite LuAl defect-related trap in Lu3Al5O12:Ce single crystal. Phys Status Solidi B 2005, 242: R119–R121.
[19]
Liu SP, Mares JA, Babin V, et al. Composition and properties tailoring in Mg2+ codoped non-stoichiometric LuAG:Ce,Mg scintillation ceramics. J Eur Ceram Soc 2017, 37: 1689–1694.
[20]
Nikl M, Kamada K, Babin V, et al. Defect engineering in Ce-doped aluminum garnet single crystal scintillators. Cryst Growth Des 2014, 14: 4827–4833.
[21]
Nikl M, Pejchal J, Mihokova E, et al. Antisite defect-free Lu3(GaxAl1−x)5O12:Pr scintillator. Appl Phys Lett 2006, 88: 141916.
[22]
Liu SP, Feng XQ, Zhou ZW, et al. Effect of Mg2+ co-doping on the scintillation performance of LuAG:Ce ceramics. Phys Status Solidi-R 2014, 8: 105–109.
[23]
Liu SP, Mares JA, Feng XQ, et al. Towards bright and fast Lu3Al5O12:Ce,Mg optical ceramics scintillators. Adv Opt Mater 2016, 4: 731–739.
[24]
Zhang JY, Luo ZH, Liu YF, et al. Cation-substitution induced stable GGAG:Ce3+ ceramics with improved optical and scintillation properties. J Eur Ceram Soc 2017, 37: 4925–4930.
[25]
Zorenko Y, Gorbenko V, Konstankevych I, et al. Single-crystalline films of Ce-doped YAG and LuAG phosphors: Advantages over bulk crystals analogues. J Lumin 2005, 114: 85–94.
[26]
Zorenko Y, Gorbenko V, Voloshinovskii A, et al. Exciton-related luminescence in LuAG:Ce single crystals and single crystalline films. Phys Status Solidi A 2005, 202: 1113–1119.
[27]
Hu ZW, Chen XP, Chen HH, et al. Suppression of the slow scintillation component of Pr:Lu3Al5O12 transparent ceramics by increasing Pr concentration. J Lumin 2019, 210: 14–20.
[28]
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.
[29]
Wang HM, Huang ZY, Qi JQ, et al. A new methodology to obtain the fracture toughness of YAG transparent ceramics. J Adv Ceram 2019, 8: 418–426.
[30]
Chen XP, Hu ZW, Dai JW, et al. Fabrication and optical properties of cerium doped Lu3Ga3Al2O12 scintillation ceramics. Opt Mater 2018, 85: 121–126.
[31]
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.
[32]
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.
[33]
Pan LJ, Jiang BX, Fan JT, et al. Preparation of LuAG powders with single phase and good dispersion for transparent ceramics using co-precipitation method. Materials 2015, 8: 5363–5375.
[34]
Milisavljevic I, Pitcher MJ, Li JQ, et al. Crystallization of glass materials into transparent optical ceramics. Int Mater Rev 2022, 1–29.
[35]
Alahraché S, Al Saghir K, Chenu S, et al. Perfectly transparent Sr3Al2O6 polycrystalline ceramic elaborated from glass crystallization. Chem Mater 2013, 25: 4017– 4024.
[36]
Allix M, Alahrache S, Fayon F, et al. Highly transparent BaAl4O7 polycrystalline ceramic obtained by full crystallization from glass. Adv Mater 2012, 24: 5570– 5575.
[37]
Boyer M, Yang XY, Carrion AJF, et al. First transparent oxide ion conducting ceramics synthesized by full crystallization from glass. J Mater Chem A 2018, 6: 5276–5289.
[38]
Boyer M, Carrion AJF, Ory S, et al. Transparent polycrystalline SrREGa3O7 melilite ceramics: Potential phosphors for tuneable solid state lighting. J Mater Chem C 2016, 4: 3238–3247.
[39]
Ma XG, Li XY, Li JQ, et al. Pressureless glass crystallization of transparent yttrium aluminum garnet-based nanoceramics. Nat Commun 2018, 9: 1175.
[40]
Zhang Y, Ma XG, Li XY, et al. Crystallization kinetics of Al2O3–26mol% Y2O3 glass and full crystallized transparent Y3Al5O12-based nanoceramic. J Eur Ceram Soc 2021, 41: 1557–1563.
[41]
Zhang Q, Zheng RL, Ding JY, et al. High lumen density of Al2O3–LuAG:Ce composite ceramic for high-brightness display. J Am Ceram Soc 2021, 104: 3260–3268.
[42]
Luo ZH, Jiang HC, Jiang J, et al. Microstructure and optical characteristics of Ce:Gd3(Ga,Al)5O12 ceramic for scintillator application. Ceram Int 2015, 41: 873–876.
[43]
Wu HY, Yang C, Zhang ZX, et al. Photoluminescence and thermoluminescence of Ce3+ incorporated Y3Al5O12 synthesized by rapid combustion. Optik 2016, 127: 1368–1371.
[44]
Liu SP, Feng XQ, Mares JA, et al. Optical, luminescence and scintillation characteristics of non-stoichiometric LuAG: Ce ceramics. J Lumin 2016, 169: 72–77.
[45]
Vedda A, di Martino D, Martini M, et al. Thermoluminescence of Zr-codoped Lu3Al5O12:Ce crystals. Phys Status Solidi A 2003, 195: R1–R3.
[46]
Liu SP, Feng XQ, Shi Y, et al. Fabrication, microstructure and properties of highly transparent Ce3+:Lu3Al5O12 scintillator ceramics. Opt Mater 2014, 36: 1973–1977.
[47]
Mao RH, Zhang LY, Zhu RY. Optical and scintillation properties of inorganic scintillators in high energy physics. IEEE Trans Nucl Sci 2008, 55: 2425–2431.
[48]
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.
[49]
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.
[50]
Han JJ, Wang Z, Li JQ, et al. Large-sized La2O3–TiO2 high refractive glasses with low SiO2 fraction by hot-press sintering. Int J Appl Glass Sci 2019, 10: 371–377.
[51]
Li RY, Li XY, Li JQ, et al. Large-sized La2O3–TiO2–SiO2 amorphous oxide fabricated by hot press sintering. J Inorg Mater 2017, 32: 851–856. (in Chinese)
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Publication history

Received: 23 June 2022
Revised: 01 October 2022
Accepted: 18 October 2022
Published: 29 December 2022
Issue date: February 2023

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© The Author(s) 2022.

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. This work has benefited from the electron microscopy facilities of the Platform MACLE-CVL, which was cofounded by the European Union and Centre-Val de Loire Region (FEDER).

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