Transparent Ce:lutetium aluminum garnet(Ce:Lu_(3)A_(l5)O_(12),Ce:LuAG)ceramics have been regarded as potential scintillator materials due to their relatively high density and atomic number(Zeff).However,the current Ce...Transparent Ce:lutetium aluminum garnet(Ce:Lu_(3)A_(l5)O_(12),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–Al_(2)O_(3) nanoceramics through the crystallization of 72 mol%Al_(2)O_(3)–28 mol%Lu_(2)O_(3)(ALu28)bulk glass.The biphasic nanostructure composed of LuAG and Al_(2)O_(3) nanocrystals makes up the whole ceramic materials.Most of Al_(2)O_(3) is distributed among LuAG grains,and the rest is present inside the LuAG grains.Fully dense biphasic LuAG–Al_(2)O_(3) 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–Al_(2)O_(3) nanoceramics with 0.3–1.0 at%Ce.The light yield of 0.3 at%Ce:LuAG–Al_(2)O_(3) nanoceramics is estimated to be 20,000 ph/MeV with short 1μs shaping time,which is far superior to that of commercial Bi_(4)Ge_(3)O_(12)(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.展开更多
Ce doped Lu_(3)Al_(5)O_(12)(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...Ce doped Lu_(3)Al_(5)O_(12)(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)_(3)Al_(5)O_(12)–Al_(2)O_(3)(LuGAG–Al_(2)O_(3))nanoceramics with different replacing contents of Gd^(3+)(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 Al_(2)O_(3) phase,exhibiting eminent transparency of 81.0%@780 nm.After doping by Ce^(3+),the Ce:LuGAG–Al_(2)O_(3) 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–Al_(2)O_(3) nanoceramics with 20%Gd^(3+)show high internal quantum efficiency(81.5%in internal quantum efficiency(IQE),96.7%of Ce:LuAG–Al_(2)O_(3) nanoceramics)and good thermal stability(only 9%loss in IQE at 150℃).When combined with blue LED chips(10 W),0.3%Ce:LuGAG–Al_(2)O_(3) nanoceramics with 20%Gd^(3+)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–Al_(2)O_(3) nanoceramics are excited by blue laser(5 W·mm^(−2)),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%Gd^(3+)).Taking into account the high quantum efficiency,good thermal stability,and excellent and adjustable luminous properties,the transparent Ce:LuGAG–Al_(2)O_(3) nanoceramics with different Gd^(3+)substitution contents in this paper are believed to be promising candidates for high-power white LED/LD lighting.展开更多
基金supported by the National Natural Science Foundation of China (No.51972304)Beijing Municipal Science&Technology Commission,Administrative Commission of Zhongguancun Science Park (No.Z221100006722022)+1 种基金the Project of Scientific Experiment on Chinese Manned Space Station,Chinese Academy of Sciences President’s International Fellowship Initiative for 2021 (No.2021VEA0012)the Fundamental Research Funds for the Central Universities.
文摘Transparent Ce:lutetium aluminum garnet(Ce:Lu_(3)A_(l5)O_(12),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–Al_(2)O_(3) nanoceramics through the crystallization of 72 mol%Al_(2)O_(3)–28 mol%Lu_(2)O_(3)(ALu28)bulk glass.The biphasic nanostructure composed of LuAG and Al_(2)O_(3) nanocrystals makes up the whole ceramic materials.Most of Al_(2)O_(3) is distributed among LuAG grains,and the rest is present inside the LuAG grains.Fully dense biphasic LuAG–Al_(2)O_(3) 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–Al_(2)O_(3) nanoceramics with 0.3–1.0 at%Ce.The light yield of 0.3 at%Ce:LuAG–Al_(2)O_(3) nanoceramics is estimated to be 20,000 ph/MeV with short 1μs shaping time,which is far superior to that of commercial Bi_(4)Ge_(3)O_(12)(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.
基金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)+1 种基金the Project of Scientific Experiment on Chinese Manned Space Station,Chinese Academy of Sciences President’s International Fellowship Initiative for 2021(No.2021VEA0012)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).Declaration of competing interest。
文摘Ce doped Lu_(3)Al_(5)O_(12)(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)_(3)Al_(5)O_(12)–Al_(2)O_(3)(LuGAG–Al_(2)O_(3))nanoceramics with different replacing contents of Gd^(3+)(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 Al_(2)O_(3) phase,exhibiting eminent transparency of 81.0%@780 nm.After doping by Ce^(3+),the Ce:LuGAG–Al_(2)O_(3) 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–Al_(2)O_(3) nanoceramics with 20%Gd^(3+)show high internal quantum efficiency(81.5%in internal quantum efficiency(IQE),96.7%of Ce:LuAG–Al_(2)O_(3) nanoceramics)and good thermal stability(only 9%loss in IQE at 150℃).When combined with blue LED chips(10 W),0.3%Ce:LuGAG–Al_(2)O_(3) nanoceramics with 20%Gd^(3+)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–Al_(2)O_(3) nanoceramics are excited by blue laser(5 W·mm^(−2)),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%Gd^(3+)).Taking into account the high quantum efficiency,good thermal stability,and excellent and adjustable luminous properties,the transparent Ce:LuGAG–Al_(2)O_(3) nanoceramics with different Gd^(3+)substitution contents in this paper are believed to be promising candidates for high-power white LED/LD lighting.