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本文主要以具有六方相结构的NaLuF ₄:Yb ³⁺/Ho ³⁺/Ce ³⁺纳米晶体为核, 采用外延生长法构建具有同质结构的NaLuF ₄:Yb ³⁺/Ho ³⁺/Ce ³⁺@NaLuF ₄:Yb ³⁺核壳纳米晶体. 借助X-射线衍射仪及透射电子显微镜对样品的晶体结构、形貌及尺寸进行表征. 在近红外光980 nm激光激发下, 通过构建核壳结构及有效调控外壳中敏化离子Yb ³⁺离子的掺杂浓度, 实现Ho ³⁺离子在NaLuF ₄纳米晶体中的红光发射增强. 实验结果表明: 在相同的激发条件下, 具有核壳结构的NaLuF ₄:Yb ³⁺/Ho ³⁺/Ce ³⁺@NaLuF ₄:Yb ³⁺纳米晶体的红光发射均得到了增强, 同时, 当外壳中Yb ³⁺离子的掺杂浓度为10.0%时, 其上转换红光发射强度最强, 为NaLuF ₄:Yb ³⁺/Ho ³⁺/Ce ³⁺晶体核红光发射强度的5.8倍. 根据其光谱特性及发光动力学过程, 讨论了同质壳及壳中敏化离子掺杂浓度变化对其发光特性的影响规律. 这种具有较强红光发射的核壳结构纳米晶体在生物医学、防伪编码、多色显示等领域具有较大的应用前景.

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Abstract

A series of the hexagonal-phase NaLuF ₄:20.0%Yb ³⁺/2.0%Ho ³⁺/12.0% Ce ³⁺@NaLuF ₄: x%Yb ³⁺core-shell (CS) nanocrystals with codoping different Yb ³⁺ions in the shell is successfully built by a sequential growth process. The crystal structures and morphologies of samples are characterized by X-ray diffractometer and transmission electron microscope. With the Yb ³⁺ion concentration increasing from 0% to 15% in NaLuF ₄shell, none of the crystal structures, sizes, and morphologies of the samples changes obviously because of the similarity in ionic radius between Yb ³⁺and the ions in shell and the low doping concentration. Under 980 nm near-infrared (NIR) excitation, the NaLuF ₄:20.0%Yb ³⁺/2.0%Ho ³⁺/12.0%Ce ³⁺core nanocrystal produce green and red UC emission. And the red UC emission intensity is higher than green emission intensity. This is because two effective cross-relaxation processes happen between Ho ³⁺and Ce ³⁺ions, which results in the enhancement of the red emission. However, the overall emission intensity of NaLuF ₄:20.0%Yb ³⁺/2.0%Ho ³⁺/12.0%Ce ³⁺nanocrystal decrease compared with that of the NaLuF ₄:20.0%Yb ³⁺/2.0%Ho ³⁺nanocrystal. Thus, to further enhance the red UC emission intensity in NaLuF ₄:20.0%Yb ³⁺/2.0%Ho ³⁺/12.0%Ce ³⁺nanocrystal, the NaLuF ₄:20.0%Yb ³⁺/2.0% Ho ³⁺/12.0%Ce ³⁺@NaLuF ₄: x%Yb ³⁺CS nanocrystal are prepared for blocking the excitation and emission energy, transmitting surface quenching center and getting more excitation energy through doping Yb ³⁺ions in NaLuF ₄shell. It can be clearly seen that the red UC emission intensity of CS nanocrystal first increases and then decreases with Yb ³⁺ion concentration increasing. Meanwhile, the corresponding red-to-green ratio increases from 4.9 to 5.6. The highest red UC emission intensity is observed in each of the NaLuF ₄:20.0%Yb ³⁺/2.0%Ho ³⁺/12.0%Ce ³⁺@NaLuF ₄:10%Yb ³⁺CS nanocrystal because the Ho ³⁺ions get more energy through the following three ways: 1) Yb ³⁺(core)-Ho ³⁺(core); 2) Yb ³⁺(shell)-Ho ³⁺(core); 3) Yb ³⁺(shell)-Yb ³⁺(core)-Ho ³⁺(core). Thus, building CS nanocrystals is one of the most effective approaches in order to improve the UC efficiency by suppressing the non-radiative decay of activators in the core and getting more excitation energy through different energy transfer ways. These NaLuF ₄:20.0%Yb ³⁺/2.0%Ho ³⁺/12.0%Ce ³⁺@NaLuF ₄:Yb ³⁺CS nanocrystals with red UC emission have great potential applications in biological field and multi-primary color.

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作者及机构信息

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

基金项目:国家自然科学基金(批准号: 11604262)、陕西省科技厅面上项目(批准号: 2018JM1052)、陕西省科技新星项目(批准号: 2019KJXX-058)、陕西省教育厅项目(批准号: 18JK0046)和宝鸡文理学院院级重点项目(批准号: ZK2018054)资助的课题

Authors and contacts

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

Funds:Project supported by the National Science Foundation of China (Grant No. 11604262), the Natural Science Basic Research Plan in Shaanxi Province of China (Grant No. 2018JM1052), Shaanxi Provincial Research Plan for Young Scientific and Technological New Stars, China (Grant No. 2019KJXX-058), the Scientific Research Program Funded by Shaanxi Provincial Education Department, China (Grant No. 18JK0046), and the Key Program of the Scientific Research of Baoji University of Arts and Sciences, China (Grant No. ZK2018054)

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参考文献

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施引文献

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Samples	CIE chromaticity coordinates
Samples	x	y
a (NaLuF₄:20.0%Yb³⁺/2.0%Ho^{3+ /}12.0%Ce³⁺)	0.5501	0.3891
b (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄)	0.5621	0.3786
c (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄: 5.0%Yb³⁺)	0.5643	0.3727
d (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄: 10.0%Yb³⁺)	0.5724	0.3692
e (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄: 15.0%Yb³⁺)	0.5756	0.3599

下载: 导出CSV

Samples	Lifetime/μs
Samples	650 nm
a (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺12.0%Ce³⁺)	97.4 ± 0.2
b (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄)	125.4 ± 1.1
c (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄:5.0%Yb³⁺)	136.3 ± 0.8
d (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄:10.0%Yb³⁺)	184.2 ± 0.6
e (NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄:15.0%Yb³⁺)	144.4 ± 0.4

下载: 导出CSV

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