单颗粒NaYF<sub>4</sub>核壳结构的能量传递特性

高伟; 张晶晶; 韩珊珊; 邢宇; 邵琳; 陈斌辉; 韩庆艳; 严学文; 张成云; 董军

doi:10.7498/aps.71.20221454

摘要

基于晶体外延生长技术构建稀土掺杂的微纳米核壳结构, 不仅有利于增强稀土离子的发射强度, 且可通过对离子的空间分离实现其发光颜色的精细调控. 为此, 本工作巧妙地借助外延生长技术构建了一系列掺杂不同离子浓度的NaYF₄@NaYF₄核壳结构微米晶体. 在980 nm近红外光激发下, 借助共聚焦显微光谱测试系统, 通过改变激发位置, 研究了掺杂离子在单颗粒核壳微米晶体中的能量传递特性. 研究表明, 当改变其激发位置时, 核壳微米盘不同区域掺杂的离子均展现出了不同的光谱特性, 其原因主要是由于在核壳结构中激发能传递方向不同所致. 基于其不同位置发射光谱及功率变化光谱, 证实微米核壳的激发能量主要是由外向内传递. 同时依据相应的光波导模型, 揭示了核壳结构微米盘多彩发射图案的产生. 由此可见, 通过构建不同微米核壳结构, 不仅能实现微米晶体发光特性的可控调节, 而且为进一步拓展微米晶体在光电子器件、光学编码及多色显示等领域中的应用提供重要的实验参考.

关键词:

Abstract

The rare-earth doped micro/nano core-shell structure not only is beneficial to enhancing the upconversion emission intensity, but also can realize the fine control of luminescence color through the spatial separation of ions. In this work, a series of NaYF₄@NaYF₄ core-shell (CS) microcrystals doped with different ion concentrations is constructed by using the epitaxial growth technology. The structure and morphology for each of the prepared microcrystals are characterized by X-ray diffractometer (XRD) and scanning electron microscope (SEM). The experimental results show that the prepared CS structures each have a pure hexagonal-phase crystal structure, and exhibit a disk-like shape. Under the excitation of 980 nm laser, the energy transfer characteristics of doped ions in single CS microcrystal are carefully studied by using a confocal microscope spectroscopy test system and changing the excitation position. The study shows that the ions doped in different regions of the CS microdisks exhibit different spectral characteristics when the excitation position is changed, which is mainly due to the different directions of excitation energy transfer in the CS structure. Based on the emission spectra of different positions and power variation spectra, it is proved that the excitation energy of the micron CS is mainly transmitted from outside to inside. Meanwhile, the colorful emission pattern of the CS microdisk is revealed by the corresponding optical waveguide model, which is mainly due to the optical waveguide effect. Therefore, by constructing different micron core-shell structures, the luminescence characteristics of microcrystals can be controlled and adjusted, which can provide important experimental reference for the applications of microcrystals in optoelectronic devices, optical coding and multicolor display.

Keywords:

作者及机构信息

西安邮电大学电子工程学院, 西安　710121

通信作者: 高伟, gaowei@xupt.edu.cn ; 董军, dongjun@xupt.edu.cn

基金项目: 国家自然科学基金(批准号: 12004304, 12104366)、陕西省重点研发项目(批准号: 2022SF-333)、陕西省青年科技新星项目(批准号: 2021KJXX-45)、陕西省自然科学基金重点项目(批准号: 2022JZ-05)、陕西省自然科学基金青年基金(批准号: 2022JQ-041)和西安邮电大学研究生创新基金(批准号: CXJJDL2021002)资助的课题.

Authors and contacts

School of Electronic Engineering, Xi’an University of Posts & Telecommunications, Xi’an 710121, China

Corresponding author: Gao Wei, gaowei@xupt.edu.cn ; Dong Jun, dongjun@xupt.edu.cn

Funds: Project supported by the National Science Foundation of China (Grant Nos. 12004304, 12104366 ), the Key R & D Program of Shaanxi Province, China (Grant No. 2022SF-333), the Shaanxi Provincial Research Plan for Young Scientific and Technological New Stars, China (Grant No. 2021KJXX-45), the Key Program of the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JZ-05), the Young Scientists Fund of the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JQ-041), and the Postgraduate Innovation Fund Project of Xi’an University of Posts and Telecommunications, China (Grant No. CXJJDL2021002).

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参考文献

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施引文献

图 1 微/纳米晶体借助核壳结构实现上转换发射的模型示意图

Fig. 1. Model schematic diagram of micro/nanocrystals up-conversion (UC) emission via core-shell (CS) structure.

下载: 全尺寸图片幻灯片

图 2 NaYF₄:20%Yb³⁺/2%Tm³⁺微米晶体及其包覆不同核壳结构的XRD图谱

Fig. 2. The XRD patterns of NaYF₄:20%Yb³⁺ /2%Tm³⁺ microcrystals and their coating with different CS structures.

下载: 全尺寸图片幻灯片

图 3 NaYF₄:20%Yb³⁺/2%Tm³⁺微米晶体及包覆不同核壳结构的SEM及其相应的元素映射图　(a) NaYF₄:20%Yb³⁺/2%Tm³⁺; (b) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺; (c) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺@ NaYbF₄

Fig. 3. The SEM images and element mappings of NaYF₄:20%Yb³⁺/2%Tm³⁺ microcrystals with corresponding CS structures: (a) NaYF₄:20%Yb³⁺/2%Tm³⁺; (b) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺; (c) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺@ NaYbF₄.

下载: 全尺寸图片幻灯片

图 4 共聚焦显微光谱测试系统示意图

Fig. 4. Schematic diagram of the confocal microscope spectroscopic test system.

下载: 全尺寸图片幻灯片

图 5 在980 nm激发下, 单个NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺核壳微米盘在不同激发位置的　(a)上转换发射光谱(插图为不同激发位置下对应的发光照片), (b)蓝光、绿光和红光的发射峰面积, (c)增强倍数和(d)红绿比和红蓝比

Fig. 5. (a) The UC emission spectra (The insert is corresponding optical micrographs at different excitation positions), (b) the peak area of the bule, green and red emission intensity, (c) enhancement and (d) R/G ratio and R/B ratio of the single NaYF₄:20%Yb³⁺/2%Tm³⁺@ NaYF₄:20%Yb³⁺/2%Er³⁺ CS microdisk at different excitation positions under the excitation of a 980 nm near-infrared (NIR) laser.

下载: 全尺寸图片幻灯片

图 6 在980 nm激发下, 单个NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄核-壳-壳微米盘在不同激发位置的　(a)上转换发射光谱(插图为不同激发位置下对应的发光照片), (b)蓝光、绿光和红光的发射峰面积, (c)增强倍数和(d)红绿比和红蓝比

Fig. 6. (a) The UC emission spectra (The insert is corresponding optical micrographs at different excitation positions), (b) the peak area of the bule, green and red emission intensity, (c) enhancement and (d) R/G ratio and R/B ratio of the single NaYF₄:20%Yb³⁺/2%Tm³⁺@ NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄ core-shell-shell (CSS) microdisk at different excitation positions under the excitation of a 980 nm NIR laser.

下载: 全尺寸图片幻灯片

图 7 在980 nm激发下, 单个NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄核-壳-壳微米盘中Yb³⁺, Tm³⁺和Er³⁺离子在不同核壳体系之间所对应的能级图及跃迁机制图(插图为核-壳-壳微米盘的模型, 白点、绿点、蓝点和紫点分别代表Yb³⁺离子、Er³⁺离子、Tm³⁺离子和表面猝灭点)

Fig. 7. The corresponding energy level diagrams and transition mechanism diagrams of Yb³⁺, Tm³⁺ and Er³⁺ ions between different CS systems in a single NaYF₄:20%Yb³⁺/2%Tm³⁺@ NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄ CSS microdisk under the excitation of a 980 nm NIR laser. (The inset is a model of a CSS microdisk, and the white, green, blue, and purple dots represent Yb³⁺ ions, Er³⁺ ions, Tm³⁺ ions, and surface quenching points, respectively.)

下载: 全尺寸图片幻灯片

图 8 在980 nm不同激发功率下, 单个(a) NaYF₄:20%Yb³⁺/2%Tm³⁺和(c) NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺微米盘在激发位置d的上转换发射光谱(插图为其对应的发光照片); (b), (d) 其蓝光, 绿光和红光发射强度与泵浦功率间的依赖关系

Fig. 8. The UC emission spectra of a single (a) NaYF₄:20%Yb³⁺/2%Tm³⁺ and (c) NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺ microdisk at excitation position d under different excitation powers of a 980 nm NIR laser (The insert is corresponding optical micrographs); (b), (d) the dependence of its blue, green and red emission intensity on pump power.

下载: 全尺寸图片幻灯片

图 9 (a)—(d) 在980 nm激发下, 单个NaYF₄:Yb³⁺/Tm³⁺@NaYF₄:Yb³⁺/Er³⁺@NaYbF₄核-壳-壳微米盘分别在激发位置a, b, c, d的发光图案及其光波导模型

Fig. 9. (a)–(d) The Luminescence patterns and optical waveguide models of a single NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄ CSS microdisk at excitation positions a, b, c, d respectively under the excitation of a 980 nm NIR laser.

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表 1 水热法制备微米晶体的药品详细参数

Table 1. Detailed parameters of medicines for the preparation of microcrystals by hydrothermal method.

样品	核(核/壳)体积/mL	m(EDTA-2Na)/g	V(RE(NO₃)₃)/mL	V(NaF) /mL
NaYF₄:Yb³⁺/Tm³⁺	—	0.282	1.5	11.0
NaYF₄:Yb³⁺/Tm³⁺@NaYF₄:Yb³⁺/Er³⁺	5.0	0.282	1.5	11.0
NaYF₄:Yb³⁺/Tm³⁺@NaYF₄:Yb³⁺/Er³⁺@NaYbF₄	5.0	0.282	1.5	11.0
注: RE(NO₃)₃和NaF溶液均为0.5 mol/L水溶液.

下载: 导出CSV

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[11]	Dong H, Sun L D, Yan C H 2021 J. Am. Chem. Soc. 143 20546 Google Scholar
[12]	Wang J, Sun X Y, Han Y D, Cheng Z Z, Liu T G 2021 Opt. Commun. 483 126663 Google Scholar
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单颗粒NaYF₄核壳结构的能量传递特性

Energy transfer characteristics of single-particle NaYF₄ core-shell structure

摘要

Abstract

作者及机构信息

西安邮电大学电子工程学院, 西安　710121

通信作者: 高伟, gaowei@xupt.edu.cn ; 董军, dongjun@xupt.edu.cn

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School of Electronic Engineering, Xi’an University of Posts & Telecommunications, Xi’an 710121, China

Corresponding author: Gao Wei, gaowei@xupt.edu.cn ; Dong Jun, dongjun@xupt.edu.cn

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单颗粒NaYF4核壳结构的能量传递特性

Energy transfer characteristics of single-particle NaYF4 core-shell structure

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Abstract

作者及机构信息

西安邮电大学电子工程学院, 西安 710121

通信作者: 高伟, gaowei@xupt.edu.cn ; 董军, dongjun@xupt.edu.cn

Authors and contacts

School of Electronic Engineering, Xi’an University of Posts & Telecommunications, Xi’an 710121, China

Corresponding author: Gao Wei, gaowei@xupt.edu.cn ; Dong Jun, dongjun@xupt.edu.cn

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单颗粒NaYF₄核壳结构的能量传递特性

Energy transfer characteristics of single-particle NaYF₄ core-shell structure

西安邮电大学电子工程学院, 西安　710121