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).

文章全文 : translate this paragraph

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.

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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

map

[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
[6]	严学文, 王朝晋, 王博扬, 孙泽煜, 张晨雪, 韩庆艳, 祁建霞, 董军, 高伟 2019 68 174204 Google Scholar Yan X W, Wang C J, Wang B Y, Sun Z Y, Zhang C X, Han Q Y, Qi J X, Dong J, Gao W 2019 Acta Phys. Sin. 68 174204 Google Scholar
[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
[9]	Wang W, Feng Z, Li B, Chang Y L, Li X, Yan X, Chen R Z, Yu X M, Zhao H Y, Lu G Y, Kong X G, Qian J, Liu X M 2021 J. Mater. Chem. B 9 2899 Google Scholar
[10]	Xu F, Sun Y, Gao H P, Jin S Y, Zhang Z L, Zhang H F, Pan G C, Kang M, Ma X Q, Mao Y L 2021 ACS Appl. Mater. Interfaces 13 2674 Google Scholar
[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
[13]	Lin H, Xu D K, Li A M, Teng D D, Yang S H, Zhang Y L 2016 Sci. Rep. 6 28051 Google Scholar
[14]	Lin H, Xu D K, Li A M, Qiu Z R, Yang S H, Zhang Y L 2017 New J. Chem. 41 1193 Google Scholar
[15]	Seki K, Uematsu K, Toda K, Sato M 2014 Chem. Lett. 43 1213 Google Scholar
[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
[19]	Lin H, Cheng Z Y, Xu D K, Zhang X G, Ge J, Xu L Q, Ma Y, Yang S H, Zhang Y L 2021 J. Mater. Chem. C 9 4385 Google Scholar
[20]	Lin H, Xu D K, Cheng Z Y, Li Y G, Xu L Q, Ma Y, Yang S H, Zhang Y L 2020 Appl. Surf. Sci. 514 146074 Google Scholar
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[26]	Choi J E, Kim D, Jang H S 2019 Chem. Commun. 55 2261 Google Scholar
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[28]	Xie X Y, Li Q Q, Chen H R, Wang W, Wu F X, Tu L P, Zhang Y L, Kong X G, Chang Y L 2022 Nano Lett. 22 5339 Google Scholar
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[41]	董军, 张晨雪, 程小同, 邢宇, 韩庆艳, 严学文, 祁建霞, 刘继红, 杨祎, 高伟 2021 70 154208 Google Scholar Dong J, Zhang C X, Cheng X T, Xing Y, Han Q Y, Yan X W, Qi J X, Liu J H, Yang Y, Gao W 2021 Acta Phys. Sin. 70 154208 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