高功率激光照明用Al2O3-YAG:Ce复相陶瓷荧光体的组分设计与性能优化

doi:10.15541/jim20220249

无机材料学报 ›› 2022, Vol. 37 ›› Issue (12): 1358-1364.DOI: 10.15541/jim20220249 CSTR: 32189.14.10.15541/jim20220249

高功率激光照明用Al₂O₃-YAG:Ce复相陶瓷荧光体的组分设计与性能优化

程梓秋¹^,²(), 王雁斌¹^,³, 刘欣¹^,², 代正发¹^,², 陈昊鸿¹^,², 田丰¹^,², 陈鹏辉¹^,², 李江¹^,²()

1.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
2.中国科学院大学材料科学与光电工程中心, 北京 100049
3.江苏大学材料科学与工程学院, 镇江 212013

收稿日期:2022-04-26 修回日期:2022-05-18 出版日期:2022-12-20 网络出版日期:2022-08-26
通讯作者: 李江, 研究员. E-mail: lijiang@mail.sic.ac.cn
作者简介:程梓秋(1998-), 男, 硕士研究生. E-mail: chengziqiu20@mails.ucas.ac.cn

Component Regulation and Performance Optimization of Al₂O₃-YAG:Ce Composite Ceramic Phosphors for High-power Laser Lighting

CHENG Ziqiu¹^,²(), WANG Yanbin¹^,³, LIU Xin¹^,², DAI Zhengfa¹^,², CHEN Haohong¹^,², TIAN Feng¹^,², CHEN Penghui¹^,², LI Jiang¹^,²()

1. Key Laboratory of Transparent Opto-Functional Inorganic Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China
2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China
3. School of Material Science and Engineering, Jiangsu University, Zhenjiang 212013, China

Received:2022-04-26 Revised:2022-05-18 Published:2022-12-20 Online:2022-08-26
Contact: LI Jiang, professor. E-mail: lijiang@mail.sic.ac.cn
About author:CHENG Ziqiu (1998-), male, Master candidate. E-mail: chengziqiu20@mails.ucas.ac.cn
Supported by:
Strategic Priority Research Program of Chinese Academy of Sciences(XDA22010301)

摘要/Abstract

摘要：

结合蓝色激光二极管和黄色荧光转换器制备的固态激光照明引起了人们极大的关注, 但荧光转换材料的热猝灭效应显著影响了高功率激光照明的实现。通过组分设计和性能优化可以提高荧光转换器的热导率和发光均匀性。本工作采用固相反应烧结技术制备了一系列不同Al₂O₃含量的Al₂O₃-YAG:Ce复相陶瓷荧光体, 研究了Al₂O₃含量对Al₂O₃-YAG:Ce陶瓷荧光体微观结构、相组成、光学性能和热学性能的影响。Al₂O₃-YAG:Ce陶瓷荧光体在800 nm处的总透过率随着Al₂O₃含量的增加(0→90%)而下降(82.6%→23.6%)。Al₂O₃-YAG:Ce陶瓷荧光体的激发和发射强度随Al₂O₃含量的增加先增大后减小。当Al₂O₃/Al₂O₃-YAG:Ce的质量比为70%时, 陶瓷荧光体在室温下的热导率高达25.7 W·m^-1·K^-1, 且表现出最高的发射强度。当采用功率密度为20 W·mm^-2的蓝光二极管泵浦 70% Al₂O₃-YAG:Ce复相陶瓷荧光体时, 可获得3724 lm的高光通量和239.4 lm·W^-1的高流明效率。此外, 当功率密度从1 W·mm^-2增大到20 W·mm^-2时, 流明效率仅下降10.5%, 光通量持续增加且未出现发光饱和。上述结果显示, Al₂O₃-YAG:Ce复相陶瓷荧光体具有良好的发光效率和热稳定性, 将在高功率激光照明中具有广阔的应用前景。

关键词: Al₂O₃-YAG:Ce, 激光照明, 流明效率, 组分设计, 性能优化

Abstract:

Solid-state laser lighting fabricated by combining blue laser diodes (LDs) and yellow-emitting phosphor converters has attracted great attention in high-luminance applications. However, the achievement of high-power laser lighting is significantly affected by the thermal quenching effect of phosphor converter materials. Therefore, component regulation and performance optimization are required to improve the thermal conductivity and luminescence uniformity of phosphor converters. In this work, a series of Al₂O₃-YAG:Ce composite ceramic phosphors with different Al₂O₃ contents were prepared by solid-state reaction sintering. The influences of Al₂O₃contents on the microstructure, phase composition, optical properties and thermal performance of the Al₂O₃-YAG:Ce ceramic phosphors were investigated in detail. The total transmittance of the Al₂O₃-YAG:Ce ceramic phosphors at 800 nm tends to decline (82.6%→23.6%) with the increase of Al₂O₃ content (0→90%, weight ratio). Both excitation and emission intensity of the Al₂O₃-YAG:Ce ceramic phosphors initially increase and then decrease with increasing Al₂O₃ content. When the weight ratio of Al₂O₃/Al₂O₃-YAG:Ce is 70%, the ceramic phosphor exhibits a high thermal conductivity of 25.7 W·m^-1·K^-1 at room temperature and the highest emission intensity. A high luminous flux of 3724 lm and luminous efficacy of 239.4 lm·W^-1 are obtained when pumping the 70% Al₂O₃-YAG:Ce ceramic phosphor with blue LDs at a power density of 20 W·mm^-2. Additionally, the luminous efficacy only decreases by 10.5% and the luminous flux continues to increase without showing luminescence saturation, when the power density increases from 1 W·mm^-2 to 20 W·mm^-2. Therefore, the Al₂O₃-YAG:Ce composite ceramic phosphors are promising in high-power laser lighting for excellent luminous efficiency and improved thermal stability.

Key words: Al₂O₃-YAG:Ce, laser lighting, luminous efficacy, component regulation, performance optimization

中图分类号:

TQ174

程梓秋, 王雁斌, 刘欣, 代正发, 陈昊鸿, 田丰, 陈鹏辉, 李江. 高功率激光照明用Al₂O₃-YAG:Ce复相陶瓷荧光体的组分设计与性能优化[J]. 无机材料学报, 2022, 37(12): 1358-1364.

CHENG Ziqiu, WANG Yanbin, LIU Xin, DAI Zhengfa, CHEN Haohong, TIAN Feng, CHEN Penghui, LI Jiang. Component Regulation and Performance Optimization of Al₂O₃-YAG:Ce Composite Ceramic Phosphors for High-power Laser Lighting[J]. Journal of Inorganic Materials, 2022, 37(12): 1358-1364.

图/表 6

Fig. 1 Photograph of xAl2O3-YAG:Ce ceramic phosphors with thickness of 1 mm

Fig. 2 XRD patterns of xAl2O3-YAG:Ce ceramic phosphors

Fig. 3 SEM images of xAl2O3-YAG:Ce ceramic phosphors (a) x=20%, (b) x=40%, (c) x=60%, and (d) x=70% thermally etched at 1450 ℃ for 3 h in air

Fig. 4 Total transmittance of xAl2O3-YAG:Ce ceramic phosphors (a) Total transmittance curves; (b) Total transmittance at 800 nmColor figures can be obtained from online edition

Fig. 5 PL and PLE spectra of xAl2O3-YAG:Ce ceramic phosphors (a) PL and PLE spectra; (b) PL and PLE spectra intensity at 465 and 550 nmColor figures can be obtained from online edition

Fig. 6 Light propagation path, luminous efficacy, luminous flux and thermal conductivity of xAl2O3-YAG:Ce ceramic phosphors (a) Diagram of reflection mode to measure luminous properties and light propagation; (b) Luminous efficacy of the ceramics with different Al2O3 contents under 1 W·mm-2 blue laser irradiation; (c) Luminous efficacy and luminous flux of 70% Al2O3-YAG:Ce as a function of blue laser power density; (d) Thermal conductivity of 70% Al2O3-YAG:Ce as a function of temperature from 25 ℃ to 300 ℃

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高功率激光照明用Al₂O₃-YAG:Ce复相陶瓷荧光体的组分设计与性能优化

Component Regulation and Performance Optimization of Al₂O₃-YAG:Ce Composite Ceramic Phosphors for High-power Laser Lighting

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