高亮度固态照明用LuYAG∶Ce荧光陶瓷(英文)_黄新友.pdf
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1、第 44 卷 第 6 期2023年 6 月Vol.44 No.6June,2023发光学报CHINESE JOURNAL OF LUMINESCENCELuYAG Ce Transparent Ceramic Phosphors for High-brightness Solid-state Lighting ApplicationHUANG Xinyou1,WANG Yanbin1,2,CHENG Ziqiu2,3,CHEN Haohong2,3,DAI Zhengfa2,TIAN Feng2,3,CHEN Penghui2,3,HU Song2,3,ZHOU Guohong2,3,LI J
2、iang2,3*(1.School of Material Science and Engineering,Jiangsu University,Zhenjiang 212013,China;2.Transparent Ceramics Research Center,Shanghai Institute of Ceramics,Chinese Academy of Sciences,Shanghai 201899,China;3.Center of Materials Science and Optoelectronics Engineering,University of Chinese
3、Academy of Sciences,Beijing 100049,China)*Corresponding Author,E-mail:lijiang Abstract:Achieving high luminous efficiency,high brightness and good thermal stability is an urgent requirement for solid-state lighting.Therefore,the high-performance color converters for high-power light-emitting diodes
4、or laser diodes(LEDs/LDs)are significant to be explored.In this work,an effective strategy to improve the luminescent properties of YAG Ce color converters through method of component regulation was realized in YAGCe transparent ceramic phosphors(TCPs)by incorporating Lu3+ions.We prepared(Lu,Y)3Al5O
5、12Ce TCPs(LuYAG Ce TCPs)with different Lu3+contents by the solid-state reaction and vacuum sintering method.With the increase of Lu3+content,the Y3+sites in LuYAG Ce TCPs were substituted by Lu3+sites,and the emission peaks of Ce3+were blue-shifted from 573 nm to 563 nm.When the Lu3+content was 60%,
6、the emission intensity reached the maximum value and the luminous efficiency reached 114 lmW-1 by combining the LuYAG Ce TCPs with a blue LED.A 450 nm laser source was used to construct a laser-driven lighting device in a transmission mode.As the power density increased from 2.2 Wmm-2 to 39 Wmm-2,th
7、e luminous flux of the TCP with 60%Lu3+substitution increased from 128 lm to 1 874 lm with no signs of luminescence saturation and the optimum luminous efficiency reached 128 lm W-1.Thus,the LuYAG Ce TCPs are expected to be potential color conversion materials for high-power LEDs/LDs lighting.Key wo
8、rds:(Lu,Y)3Al5O12Ce transparent ceramic phosphors(TCPs);solid-state lighting;color conversion materials;high-brightnessCLC number:O482.31 Document code:A DOI:10.37188/CJL.20220435高亮度固态照明用 LuYAG Ce荧光陶瓷黄新友1,王雁斌1,2,程梓秋2,3,陈昊鸿2,3,代正发2,田丰2,3,陈鹏辉2,3,胡松2,3,周国红2,3,李江2,3*(1.江苏大学 材料科学与工程学院,江苏 镇江212013;2.中国科学院
9、上海硅酸盐究所 透明陶瓷研究中心,上海201899;3.中国科学院大学 材料科学与光电工程中心,北京100049)摘要:实现高发光效率、高亮度和良好的热稳定性是固态照明的迫切要求。因此,用于高功率发光二极管或激光二极管(LED/LD)的高性能荧光转换材料具有重要的研究意义。在这项工作中,通过将 Lu3+离子引入YAG Ce荧光陶瓷中方法作为有效策略来改善 YAG Ce荧光材料的发光性能。采用固相反应和真空烧结法制Article ID:1000-7032(2023)06-0964-11收稿日期:20221231;修订日期:20230130基金项目:中国科学院战略性先导科技专项(XDA220103
10、01)Supported by The Strategic Priority Research Program of The Chinese Academy of Sciences(XDA22010301)第 6 期 HUANG Xinyou,et al.:LuYAG Ce Transparent Ceramic Phosphors for High-brightness Solid-state 备了不同 Lu3+含量的(Lu,Y)3Al5O12Ce荧光陶瓷(LuYAG Ce荧光陶瓷)。随着 Lu3+含量的增加,LuYAG Ce荧光陶瓷中的 Y3+位点被 Lu3+位点取代,Ce3+的发射峰呈现
11、从 573 nm 到 563 nm 的蓝移现象。当 Lu3+含量为 60%时,通过将 LuYAG Ce 荧光陶瓷与蓝光 LED 组合,其发光强度达到最大值,流明效率达到 114 lmW-1。使用450 nm 激光源与 LuYAG Ce荧光陶瓷构建了透射模式下的激光驱动照明装置。随着功率密度从 2.2 Wmm-2增加到 39 Wmm-2,Lu3+含量为 60%的荧光陶瓷光通量从 128 lm增加到 1 874 lm,且没有发光饱和的迹象,最佳发光效率达到 128 lmW-1。因此,LuYAG Ce荧光陶瓷有望成为高功率 LED/LD照明的潜在荧光转换材料。关键词:(Lu,Y)3Al5O12Ce荧
12、光陶瓷;固态照明;荧光转换材料;高亮度1IntroductionSolid-state lighting(SSL)owns the advantages of high brightness,high efficiency,long service life and environmental protection,which has been widely used in automobile,aviation and navigation,etc1-5.Commonly used solid-state illuminators are mainly composed of color c
13、onversion materials and blue light-emitting diodes(LEDs).Color conversion materials mainly include phosphor,phosphor in glasses(PiGs),single crystal phosphors(SCPs)and transparent ceramic phosphors(TCPs)6-7.With the development of high-brightness and high-efficiency laser diodes(LDs),thermally quenc
14、hable phosphor and PiGs are gradually substituted by SCPs and TCPs with better thermal stability8-11.Transparent ceramic phosphors possess good thermal properties and high chemical stability,as well as the advantages of adjustable microstructure and simple preparation process,which is lower cost tha
15、n SCPs11-13.The widely used yellow phosphor Y3Al5O12Ce3+(YAG Ce)TCPs can be excited to yellow light by blue light,and then the yellow light can mixed with the transmitted blue light to generate white light14-17.Component regulation of YAGCe phosphor has been proven to be a reliable strategy to impro
16、ve the luminescence performance of TCPs.For instance,introducing Gd3+,Mg2+-Si4+pairs,Sc3+and Lu3+-Sc3+pairs into YAG Ce phosphor can effectively regulate spectral characteristics and improve luminescent properties18-23.However,the increasing power density of blue LEDs and LDs put forward higher requ
17、irements on the thermal stability of YAGCe TCPs.Therefore,it is significant to obtain the YAGCe TCPs with excellent thermal stability.Lu3Al5O12 Ce3+(LuAG Ce)TCPs are also suitable for high-power SSLs,which have many advantages such as high luminous efficiency and low thermal quenching among common p
18、hosphors,but LuAG Ce TCPs require stricter sintering condition24-27.Lu3+(175)ions have a higher atomic weight than Y3+(89)ions and the 4f sublayer of Lu3+ions is completely filled with electrons,leading to the thermal stability of LuAG higher than that of YAG28-34.Therefore,replacing Y3+sites with L
19、u3+sites in YAG Ce TCPs can not only improve the thermal stability but also maintain excellent luminescent properties.At present,there are some researches about LuYAGCe TCPs.For example,Ling et al.35 prepared a series of LuYAG Ce TCPs and obtained excllent LED luminous properties.However,there are s
20、till few relevant studies about LuYAGCe TCPs and luminescent properties for LD lighting need to be further explored.In this work,we investigated the variation of crystal structure and spectral characteristics of Ce3+when Lu3+substituted Y3+into the dodecahedron site of the YAG host,which could influ
21、ence luminescent properties of LuYAG Ce TCPs,and proved that LuYAG Ce TCPs have great potential as the color converter for high-brightness SSL applications.A series of LuYAG Ce TCPs with different Lu3+contents were fabricated by solid-state reactive sintering in vacuum.The phase and microstructure o
22、f the ceramics were characterized by XRD and SEM.The in-line transmittance and PL/PLE spectra were tested.The luminous properties such as luminous flux and luminous efficiency by combining the prepared ceramics with a high-power blue LED and LD were measured.Moreover,the suitability of LuYAG Ce TCPs
23、 used as color converters for high-brightness solid-state lighting application was evaluated.965第 44 卷发光学报2ExperimentCeramic samples with the chemical formula of(Ce0.001Y0.999-xLux)3Al5O12(x=0,0.2,0.4,0.6,0.8,0.999)were prepared by high temperature solid-state reaction method.Commercial Y2O3(99.999%
24、,Shanghai Sinian metal materials Co.,Ltd),Lu2O3(99.999%,Jining Zhongkai New Materials Co.,Ltd),-Al2O3(99.99%,Fenghe Ceramic Co.,Ltd),CeO2(99.995%,Fujian Changting Golden Dragon Co.,Ltd)were used as raw materials.Above raw powders were weighed according to the stoichiometric ratio and then mixed by b
25、all milling for 12 h in ethanol,with 0.8%TEOS(99.999%,Alfa Aesar)and 0.08%MgO(99.998%,Alfa Aesar)as sintering aids.The powder mixtures were dried at 70 for 2 h,sieved through a 200-mesh screen and calcined at 600 in air for 4 h to remove the organic impurities.Then mixed powders were pressed into di
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