构建NaErF4@NaYbF4:2%Er3+核壳结构增强Er3+离子红光上转换发射

高伟; 骆一帆; 邢宇; 丁鹏; 陈斌辉; 韩庆艳; 严学文; 张成云; 董军

doi:10.7498/aps.72.20230762

摘要

构建核壳结构已被广泛应用于增强及调控稀土掺杂微/纳材料的发光性能. 本工作旨在通过构建NaErF₄@NaYbF₄:2%Er³⁺纳米核壳晶体, 实现了Er³⁺离子的红光发射增强. 实验结果表明: 当NaErF₄纳米晶体包覆NaYbF₄:2%Er³⁺活性壳时, 在980 nm激光激发下, 其Er³⁺离子的红光发射强度相比NaErF₄@NaYbF₄核壳晶体增强了1.4倍, 且红绿比由5.4提高至6.5. 同时, 当NaErF₄@ NaYbF₄:2%Er³⁺ 核壳晶体再次包覆NaYF₄惰性壳及引入微量Tm³⁺离子时, 其Er³⁺离子的红光发射强度相比于NaErF₄@NaYbF₄核壳结构分别增强了23.2和40.3倍, 且红绿比分别提高到7.5和10.2. 基于不同核壳晶体的光谱特性、离子间能量传递过程及其发光动力学, 对不同核壳晶体中Er³⁺离子的红光增强机理进行了讨论. 结果表明Er³⁺离子的红光增强主要借助高浓度Yb³⁺离子的双向能量传递及Tm³⁺离子的能量俘获效应所致, 同时NaYF₄惰性壳的包覆也有效降低纳米晶体表面猝灭效应. 本文所构建的具有高效红光发射的NaErF₄@NaYbF₄:2%Er³⁺@NaYF₄核壳纳米晶体在多彩防伪、显示及生物成像等领域中具有巨大的应用潜力.

关键词:

Abstract

Building core-shell structures are widely used to enhance and regulate the luminescence properties of rare-earth-doped micro/nano materials. In this work, a variety of different NaErF₄ core-shell and core-shell-shell nanocrystals are successfully constructed based on high temperature co-precipitation method by epitaxial growth technology. The upconversion red emission intensities of Er³⁺ ions in different core-shell structures are effectively enhanced by regulating their structures and doping ions. The experimental structures show that the constructed core-shell nanocrystals each have a hexagonal phase structure, and core-shell structure of about 40 nm. In the near infrared 980 nm laser excitation, the NaErF₄ core-shell nanocrystal shows a strong single-band red emission. And the single-band red emission intensity of Er³⁺ ions is enhanced through constructing the NaErF₄@NaYbF₄:2%Er³⁺ core-shell structure. The experimental results show that red emission intensity of Er³⁺ ions is about 1.4 times higher than that of the NaErF₄@NaYbF₄ core-shell structure by constructing the NaErF₄@NaYbF₄:2%Er³⁺ core-shell structures under 980 nm excitation, and its red/green emission intensity ratio increases from 5.4 to 6.5. Meanwhile, when NaErF₄@NaYbF₄:2%Er³⁺ core-shell structure recoats the NaYF₄ inert shell and is added with a small quantity of Tm³⁺ ions, their red emission intensities of Er³⁺ ions are 23.2 times and 40.3 times that of NaErF₄@NaYbF₄ core-shell structures, and their red/green emission intensity ratios reach 7.5 and 10.2, respectively. The red emission enhancement of Er³⁺ ions is mainly caused by bidirectional energy transfer process of high excitation energy of Yb³⁺ ions and energy trapping center of Tm³⁺ ions which effectively change the density of population of luminescent energy levels of Er³⁺ ions. Furthermore, the coated NaYF₄ inert shell also effectively weakens the surface quenching effect of nanocrystals. The mechanisms of red enhancement in different core-shell structures are discussed based on the spectral properties, the process of interion energy transfer, and luminescence kinetics. The constructed NaErF₄@NaYbF₄:2%Er³⁺@NaYF₄ core-shell structures with high-efficiency red emission in this work have great potential applications in the fields of colorful anti-counterfeiting, display and biological imaging.

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: 12274341, 12004304, 12104366)、陕西省重点研发计划(批准号: 2022SF-333)、陕西省自然基金重点项目(批准号: 2022JZ-05)、陕西省自然科学基金青年项目(批准号: 2022JQ-041)、陕西省教育厅服务地方专项计划 (批准号: 22JC-057)和西安邮电大学创新基金(批准号: CXJJY2022033)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. 12274341, 12004304, 12104366 ), the Key R & D Plan Program of Shaanxi Province, China (Grant No. 2022SF-333), the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JZ-05), the Natural Science Foundation Youth Program of Shaanxi Province, China (Grant No. 2022JQ-041), the Education Department Service Local Special Program of Shaanxi Province, China (Grant No. 22JC057), and the Innovation Fund Project of Xi’an University of Posts and Telecommunications, China (Grant No. CXJJY2022033).

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参考文献

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施引文献

图 1 NaErF₄@NaYbF₄及其包覆不同核壳结构的XRD图谱

Fig. 1. The XRD patterns of NaErF₄@NaYbF₄ and different C-S structures.

下载: 全尺寸图片幻灯片

图 2 NaErF₄@NaYbF₄及其包覆不同核壳结构的TEM和粒径分布

Fig. 2. The TEM images and size distribution of NaErF₄@NaYbF₄ and different C-S structures.

下载: 全尺寸图片幻灯片

图 3 在980 nm激发下, NaErF₄@NaYbF₄及其包覆不同核壳结构的(a)上转换发射光谱, (b)红绿比和(c)红、绿发射光积分强度

Fig. 3. (a) The UC emission spectra, (b) R/G ratio (c) red and green emission integration intensity of NaErF₄@NaYbF₄ and their coating with different C-S structures under 980 nm excitation.

下载: 全尺寸图片幻灯片

图 4 在980 nm不同激发功率下　(a)NaErF₄:0.5%Tm³⁺@NaYbF₄:2%Er³⁺@NaYF₄ C-S晶体的上转换发射光谱; (b)红、绿光发射与泵浦功率依赖关系; (c)红、绿光发射强度对比(插图为其对应的红绿比)

Fig. 4. (a) The UC emission spectra , (b) power density dependence of red and green emission, and (c) comparison of red and green emission intensity of NaErF₄:0.5%Tm³⁺@NaYbF₄:2%Er³⁺ @ NaYF₄ C-S structure under different excitation powers of 980 nm (The insert is corresponding R/G ratio).

下载: 全尺寸图片幻灯片

图 5 在980 nm激光激发下, NaErF₄@NaYbF₄及其包覆的不同核壳结构所对应的能级图及可能的跃迁机理图

Fig. 5. The corresponding energy level diagrams and possible transition mechanism diagrams of NaErF₄@ NaYbF₄ and their coating with different C-S structures under 980 nm excitation.

下载: 全尺寸图片幻灯片

图 6 在980 nm脉冲激光激发下, NaErF₄@NaYbF₄及其包覆不同核壳结构的寿命衰减曲线图

Fig. 6. The decay curves of NaErF₄@NaYbF₄ and their coating with different C-S structures under the excitation of a 980 nm pulse laser.

下载: 全尺寸图片幻灯片

[1]	Alkahtani M, Alsofyani N, Alfahd A, Almuqhim A A, Almuqhim F A, Alshehri A A, Qasem H, Hemmer P R 2021 Nanomaterials 11 284 Google Scholar
[2]	Sun T Y, Li Y H, Ho W L, Zhu Q, Chen X, Jin L M, Zhu H M, Huang B L, Lin J, Little B E, Chu S T, Wang F 2019 Nat. Commun. 10 1811 Google Scholar
[3]	Wang F, Deng R R, Wang J, Wang Q X, Han Y, Zhu H M, Chen X Y, Liu X G 2011 Nat. Mater. 10 968 Google Scholar
[4]	Wang Y B, Lei L, Ye R G, Jia G H, Hua Y J, Deng D G, Xu S Q 2021 ACS Appl. Mater. Interfaces 13 23951 Google Scholar
[5]	Bao H Q, Wang W, Li X, Liu X M, Zhang L, Yan X, Wang Y H, Wang C G, Jia X T, Sun P, Kong X G, Zhnag H, Lu G Y 2022 Adv. Optical Mater. 10 2101702 Google Scholar
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[7]	Meng Z P, Zhang S F, Wu S L 2020 J. Lumin. 227 117566 Google Scholar
[8]	Tang M, Zhu X H, Zhang Y H, Zhang Z P, Zhang Z M, Mei Q S, Zhang J, Wu M H, Liu J L, Zhang Y 2019 ACS Nano 13 10405 Google Scholar
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[11]	Tan M L, Li F, Wang X, Fan R W, Chen G Y 2020 ACS Nano 14 6532 Google Scholar
[12]	Zhang H B, Chen Z H, He Y R, Yang S Y, Wei J 2021 ACS Appl. Mater. Interfaces 4 4340
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[16]	Lin H, Xu D K, Li Y J, Yao L, Xu L Q, Ma Y, Yang S H, Zhang Y L 2018 Inorg. Chem. 57 15361 Google Scholar
[17]	Joshi R, Perala R S, Shelar S B, Ballal A, Singh B P, Ningthoujam S 2021 ACS Appl. Mater. Interfaces 13 3481 Google Scholar
[18]	Cheng Q, Sui J H, Cai W 2012 Nanoscale 4 779 Google Scholar
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构建NaErF₄@NaYbF₄:2%Er³⁺核壳结构增强Er³⁺离子红光上转换发射