高光效、大功率LEDs/LDs用Ce:YAG透明陶瓷

doi:10.15541/jim20200727

无机材料学报 ›› 2021, Vol. 36 ›› Issue (8): 883-892.DOI: 10.15541/jim20200727 CSTR: 32189.14.10.15541/jim20200727

高光效、大功率LEDs/LDs用Ce:YAG透明陶瓷

杜傲宸¹^,²(), 杜琪源³, 刘欣²^,⁴, 杨益民¹^,², 夏晨阳¹, 邹军³, 李江²^,⁴()

1.吉林建筑大学材料科学与工程学院, 长春130118
2.中国科学院上海硅酸盐研究所, 透明光功能无机材料重点实验室, 上海201899
3.上海应用技术大学理学院, 上海201418
4.中国科学院大学材料与光电研究中心, 北京 100049

收稿日期:2020-12-18 修回日期:2021-01-24 出版日期:2021-08-20 网络出版日期:2021-03-12
通讯作者: 李江, 研究员. E-mail: lijiang@mail.sic.ac.cn
作者简介:杜傲宸(1995-), 男, 硕士研究生. E-mail: duaochen@foxmail.com

Ce:YAG Transparent Ceramics Enabling High Luminous Efficacy for High-power LEDs/LDs

DU Aochen¹^,²(), DU Qiyuan³, LIU Xin²^,⁴, YANG Yimin¹^,², XIA Chenyang¹, ZOU Jun³, LI Jiang²^,⁴()

1. School of Materials Science and Engineering, Jilin Jianzhu University, Changchun 130118, China
2. Key Laboratory of Transparent Opto-functional Inorganic Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 201899, China
3. School of Science, Shanghai Institute of Technology, Shanghai, 201418, China
4. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Received:2020-12-18 Revised:2021-01-24 Published:2021-08-20 Online:2021-03-12
Contact: LI Jiang, professor. E-mail: lijiang@mail.sic.ac.cn
About author:DU Aochen (1995-), male, Master candidate. E-mail: duaochen@foxmail.com
Supported by:
National Key R&D Program of China(2017YFB0310500);Key Research Project of the Frontier Science of the Chinese Academy of Sciences(QYZDB-SSW-JSC022)

摘要/Abstract

摘要：

Ce:YAG透明陶瓷可与蓝光LEDs/LDs复合, 用于大功率白光LEDs/LDs。本研究通过调整Ce:YAG透明陶瓷的厚度和Ce³⁺的掺杂浓度, 将组装器件的发射光谱和色坐标从冷白区调整到暖白区。以高纯(≥99.99%)商业粉体α-Al₂O₃、Y₂O₃、CeO₂为原料, 采用固相反应法制备了(Ce_xY_1-_x)₃Al₅O₁₂ (x=0.0005、0.0010、0.0030、0.0050、0.0070和0.0100)透明陶瓷。陶瓷素坯在1750 ℃真空烧结20 h(真空度5.0×10^-5 Pa), 之后在马弗炉中退火1450 ℃×10 h。不同掺杂浓度Ce:YAG陶瓷(厚度分别为0.2、0.4、1.0 mm)在800 nm处的直线透过率均大于79%。Ce:YAG荧光陶瓷的热导率随着测试温度和掺杂浓度的增加而降低。采用有限元方法模拟不同厚度的Ce:YAG陶瓷和LED组装的热分布, 比较了三种封装方式的热分布。将Ce:YAG荧光陶瓷与LEDs/LDs复合, 制备出色坐标分别为(0.3319, 0.3827)和(0.3298, 0.3272)的白光, 发光效率分别为122.4和201.5 lm/W。将Ce:YAG荧光陶瓷和10、50 W商用蓝光LED芯片组合成熟灯具, 可用于商业用途。Ce:YAG透明陶瓷在大功率照明和显示的彩色转换材料应用领域极具潜力。

关键词: LEDs/LDs照明, 光致发光, Ce:YAG, 荧光陶瓷

Abstract:

Ce:YAG transparent ceramics could be combined with blue LEDs/LDs, for applications of high power white LEDs/LDs. In this study, it is found that by adjusting the thickness of Ce:YAG transparent ceramics and the doping concentration of Ce³⁺, the emission spectra and color coordinates of the assembled devices can be adjusted from the cold white region to the warm white region. (Ce_xY_1-_x)₃Al₅O₁₂ (x=0.0005, 0.0010, 0.0030, 0.0050, 0.0070 and 0.0100) transparent ceramics was fabricated by a solid state reaction method, with the high pure (≥99.99%) commercial powdersα-Al₂O₃, Y₂O₃ and CeO₂ using as raw materials. The ceramic green bodies were sintered in 1750 ℃ for 20 h under vacuum of 5.0×10^-5 Pa, and the ceramics were annealed at 1450 ℃ for 10 h in the muffle furnace. The in-line transmittance of double polished Ce:YAG ceramics is higher than 79% at 800 nm (0.2, 0.4, 1.0 mm in thickness, respectively). The thermal conductivity of Ce:YAG transparent ceramics decreases with the increase of measuring temperature and doping concentration. Thermal distribution of ceramics and LEDs with different thicknesses was simulated by the finite element method, and the thermal distributions of three packaging modes were compared. White light with chromaticity coordinates of (0.3319, 0.3827) and (0.3298, 0.3272) and luminous efficiency of 122.4 and 201.5 lm/W were prepared by combining transparent ceramics with LEDs/LDs. We combined Ce:YAG transparent ceramics and blue LEDs chips to produce 10 and 50 W mature lamps, which can be used for commercial purposes. Therefore, the Ce:YAG transparent ceramics is a highly promising color conversion material for high power lighting and displaying applications in the future.

Key words: LEDs/LDs illumination, photoluminescence, Ce:YAG, ceramic phosphor

中图分类号:

TQ174

杜傲宸, 杜琪源, 刘欣, 杨益民, 夏晨阳, 邹军, 李江. 高光效、大功率LEDs/LDs用Ce:YAG透明陶瓷[J]. 无机材料学报, 2021, 36(8): 883-892.

DU Aochen, DU Qiyuan, LIU Xin, YANG Yimin, XIA Chenyang, ZOU Jun, LI Jiang. Ce:YAG Transparent Ceramics Enabling High Luminous Efficacy for High-power LEDs/LDs[J]. Journal of Inorganic Materials, 2021, 36(8): 883-892.

图/表 12

Fig. 1 Flowchart for the preparation process of Ce:YAG transparent ceramics

Fig. 2 XRD patterns (a) of (CexY1-x)3Al5O12 transparent ceramics smashed into powder, expanded view (b) of 2θ diffraction peaks between 33.0° and 32.5°, and illustration of Ce:YAG crystalline structure and the coordinated environments (c) of YO8 dodecahedron, AlO4 tetrahedra, and AlO6 octahedra based on JCPDS #04-007-2667

Fig. 3 FESEM images of the thermally etched surfaces of (CexY1-x)3Al5O12 ceramics with different doping concentrations (a) x=0.0005; (b) x=0.0010; (c) x=0.0030; (d) x=0.0050; (e) x=0.0070; (f) x=0.0100

Fig. 4 Photographs of all (CexY1-x)3Al5O12 ceramics with orthogonally designed parameters under sunlight. All conditions (thickness and concentration) were independent and resulted in the great difference in color from light yellow to deep yellow (x=0.0005, 0.0010, 0.0030, 0.0050, 0.0070 and 0.0100, d=0.2, 0.4 and 1.0 mm)

Fig. 5 In-line transmittance curves for annealed and unannealed (CexY1-x)3Al5O12 ceramics (x=0.0005, 0.0010, 0.0030, 0.0050, 0.0070 and 0.0100, d=0.2, 0.4 and 1.0 mm)

Fig. 6 PLE and PL spectra (a) of (CexY1-x)3Al5O12 ceramics, Gaussian deconvolution (b) of the 0.5at%Ce:YAG ceramic with inset showing energy-level scheme of Ce3+, PLE (λem=525 nm) (c) and PL (λex=450 nm) (e) of the prepared Ce:YAG ceramics as the function of Ce3+ doping concentration, the detailed peak positions and emission intensities of PLE (d) and PL (f) spectra of the Ce:YAG ceramics (x=0.0005, 0.0010, 0.0030, 0.0050, 0.0070 and 0.0100)

Fig. 7 Thermal quenching behavior (a) for photoluminescence 0.50at%Ce:YAG ceramic phosphor, detailed peak positions and emission intensities of PL spectra (b) of 0.5at%Ce:YAG ceramic, thermal conductivity (c) of (CexY1-x)3Al5O12 ceramics at different temperatures, and configurational coordination diagrams (d) illustrating the thermally quenching of 5d-4f luminescence of Ce3+

Fig. 8 Simplified three-dimensional model view of assemblage and white LEDs encapsulation model (TOP figure), thermal distribution of 0.5at%Ce:YAG transparent ceramics, thickness 0.2 mm (a, d), 0.4 mm (b, e), 1.0 mm (c, f) respectively, during steady thermal state or transient thermal state, and (g-i) three common packaging methods and heat dissipation

Fig. 9 EL spectra of Ce:YAG ceramics with different doping concentrations (a) and thickness (b), CIE of the LEDs with Ce:YAG ceramics of different doping concentrations (c) and thicknesses (d), the pictures of the LEDs with Ce:YAG ceramics with the increase of doping concentrations and thickness, which changes from blue to yellow (e-g)

Fig. 10 EL spectra of Ce:YAG ceramics with different doping concentrations (a) and thicknesses (b), CIE of the LDs with Ce:YAG ceramics of different doping concentrations (c) and thicknesses (d)

Fig. 11 Packaged LEDs devices from blue to yellow arbitrarily by adjusting the Ce3+ concentration and the thickness of transparent ceramics

Table 1 White light emission parameters of Ce:YAG packaged devices ((CexY1-x)3Al5O12)

LEDs/LDs	x	Thickness/mm	LE/(lm·W^-1)	CIE	CCT/K	CRI
LED	0.0005	1.0	122.4	(0.3319, 0.3827)	5528	62.8
LED	0.0010	0.4	115.5	(0.3021, 0.3217)	7196	68.8
LED	0.0030	0.2	83.7	(0.3166, 0.3442)	6216	67.1
LD	0.0010	1.0	201.5	(0.3298, 0.3272)	7415	65.1
LD	0.0050	0.2	170.3	(0.3146, 0.3169)	7264	65.4

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高光效、大功率LEDs/LDs用Ce:YAG透明陶瓷

Ce:YAG Transparent Ceramics Enabling High Luminous Efficacy for High-power LEDs/LDs

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