Enhanced red upconversion fluorescence emission of Ho<sup>3+</sup> ions in NaLuF<sub>4</sub> nanocrystals through building core-shell structure

Yan Xue-Wen; Wang Zhao-Jin; Wang Bo-Yang; Sun Ze-Yu; Zhang Chen-Xue; Han Qing-Yan; Qi Jian-Xia; Dong Jun; Gao Wei

doi:10.7498/aps.68.20190441

Abstract

A series of the hexagonal-phase NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0% Ce³⁺@NaLuF₄:x%Yb³⁺ core-shell (CS) nanocrystals with codoping different Yb³⁺ 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 Yb³⁺ ion concentration increasing from 0% to 15% in NaLuF₄ shell, none of the crystal structures, sizes, and morphologies of the samples changes obviously because of the similarity in ionic radius between Yb³⁺ and the ions in shell and the low doping concentration. Under 980 nm near-infrared (NIR) excitation, the NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺ 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 Ho³⁺ and Ce³⁺ ions, which results in the enhancement of the red emission. However, the overall emission intensity of NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺ nanocrystal decrease compared with that of the NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺ nanocrystal. Thus, to further enhance the red UC emission intensity in NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺ nanocrystal, the NaLuF₄:20.0%Yb³⁺/2.0% Ho³⁺/12.0%Ce³⁺@NaLuF₄:x%Yb³⁺ CS nanocrystal are prepared for blocking the excitation and emission energy, transmitting surface quenching center and getting more excitation energy through doping Yb³⁺ ions in NaLuF₄ shell. It can be clearly seen that the red UC emission intensity of CS nanocrystal first increases and then decreases with Yb³⁺ 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 NaLuF₄:20.0%Yb³⁺ /2.0%Ho³⁺/12.0%Ce³⁺@NaLuF₄:10%Yb³⁺ CS nanocrystal because the Ho³⁺ ions get more energy through the following three ways: 1) Yb³⁺ (core)-Ho³⁺ (core); 2) Yb³⁺ (shell)-Ho³⁺ (core); 3) Yb³⁺ (shell)-Yb³⁺ (core)-Ho³⁺ (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 NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@NaLuF₄:Yb³⁺ CS nanocrystals with red UC emission have great potential applications in biological field and multi-primary color.

Keywords:

Authors and contacts

1.
School of Electronic Engineering, Xi’an University of Post and Telecommunications, Xi’an 710121, China
2.
College of Physics and Optoelectronics Technology, Baoji University of Arts and Sciences, Baoji 721016, China

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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References

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Cited By

图 1 (a) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺纳米晶体核, (b)−(e) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄:x%Yb³⁺(x = 0%, 5.0%, 10.0%, 15.0%)纳米核壳结构的XRD图谱

Figure 1. XRD patterns of (a) NaLuF₄:20.0%Yb³⁺ /2.0%Ho³⁺/12.0%Ce³⁺ nanocrystals and (b)−(e) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄:x%Yb³⁺(x = 0%, 5.0%, 10.0%, 15.0%) core-shell nanocrystals.

DownLoad: Full-Size Img PowerPoint

图 2 (a) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺纳米晶体和NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12%Ce³⁺@ NaLuF₄:x%Yb³⁺((b) 0, (c) 5.0%, (d)10.0%, (e) 15.0%)纳米核壳结构的TEM图谱

Figure 2. TEM images and EDX spectra of (a) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺ nanocrystals and (b)−(e) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄: x%Yb³⁺ (x = 0, 5.0%, 10.0%, 15.0%) core-shell nanocrystals.

DownLoad: Full-Size Img PowerPoint

图 3 在980 nm激发下, (a) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺和(b)−(e) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@ NaLuF₄:x%Yb³⁺ (x = 0%, 5.0%, 8.0%,10.0%, 12.0%, 15.0%)纳米晶体及核壳结构的上转换发射光谱(A)、增强因子(B)和红绿比(C)

Figure 3. The upconverison emission spectra (A), enhancement factor (B) and red andgreen emission intensity ratio (R/G) (C) of (a) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺ nanocrystals and (b)−(e) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12%Ce³⁺@ NaLuF₄:x%Yb³⁺ (x = 0%, 5.0%, 8.0%, 10.0%, 12.0%,15.0%) core-shell nanocrystals under 980 nm excitation.

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图 4 (a) NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺以及(b)—(e)NaLuF₄:20.0%Yb³⁺/2.0%Ho³⁺/12.0%Ce³⁺@NaLuF₄:x%Yb³⁺ (x = 0%, 5.0%, 10.0%, 15.0%) 纳米晶体及核壳结构的色度坐标图

Figure 4. The CIE diagram with position of color coordinates of Ho³⁺ in (a) NaLuF₄ nanocrystals and (b)－(e) NaLuF₄@ NaLuF₄:x%Yb³⁺ (x = 0%, 5.0%, 10.0%, 15.0%) core-shell nanocrystals.

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图 5 Ho³⁺, Yb³⁺和Ce³⁺离子的能级图和可能的上转换跃迁机理

Figure 5. Energy level diagrams of Ho³⁺, Yb³⁺, and Ce³⁺ions as well as proposed UC mechanisms.

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图 6 在980 nm近红外激光的激发下, Ho³⁺离子掺杂NaLuF₄和NaLuF₄@ NaLuF₄纳米晶体的红光上转换发射的寿命衰减曲线图

Figure 6. Luminescence lifetimes of NaLuF₄ and NaLuF₄@NaLuF₄ core-shell nanocrystals under 980 nm excitation at 654 nm.

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表 1 NaLuF₄和NaLuF₄@NaLuF₄核壳纳米晶体的的CIE色坐标

Table 1. The calculated CIE chromaticity coordinates (x, y) of Ho³⁺ in NaLuF₄ nanocrystals and NaLuF₄@ NaLuF₄:x%Yb³⁺ (x = 0%, 5.0%, 10.0%, 15.0%) core-shell nanocrystals.

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

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表 2 NaLuF₄和NaLuF₄@ NaLuF₄核壳纳米晶体的红光发射的荧光寿命

Table 2. Luminescence lifetimes of NaLuF₄ and NaLuF₄@NaLuF₄ core-shell nanocrystals under 980 nm excitation at 650 nm

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

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[1]	Menyuk N, Dwight K, Pinaud F 1972 Appl. Phys. Lett. 21 159 Google Scholar
[2]	Downing E, Hesselink L, Ralston J, Macfarlane R A 1996 Science 273 1185 Google Scholar
[3]	Zhang Y, Zhang L, Deng R, Tian J, Zong Y, Jin D, Liu X G 2014 J. Am. Chem. Soc. 136 4893 Google Scholar
[4]	Zou W, Visser C, Maduro J A, Pshenichnikov M S, Hummelen J C 2012 Nat. Photon. 6 560 Google Scholar
[5]	Su Q, Feng W, Yang D, Li F 2017 Acc. Chem. Res. 50 32 Google Scholar
[6]	Huang B L, Dong H, Wong K L, Sun L D, Yan C H 2016 J. Phys. Chem. C 120 18858 Google Scholar
[7]	Niu N, Yang P P, He F, Zhang X, Gai S L, Li C X, Lin J 2012 J. Mater. Chem. 2 2
[8]	高当丽, 郑海荣, 田宇, 雷瑜, 崔敏, 何恩节, 张喜生 2010 中国科学: 物理学力学天文学 40 287 Gao D L, Zheng H R, Tian Y, Lei Y, Cui M, He E J, Zhang X S 2010 Sci. Sin.: Phys. Mech. Astron. 40 287
[9]	Gao W, Zheng H R, He E J, Lu Y, Gao F Q 2014 J. Lumin. 152 44 Google Scholar
[10]	Teng X, Zhu Y H, Wei W, Wang S C, Huang J F, Naccache R, Hu W B, Tok A I Y, Han Y, Zhang Q C, Fan Q L, Huang W, Capobianco J A, Huang L 2012 J. Am. Chem. Soc. 134 8340 Google Scholar
[11]	Heer S, Kompe K, Gudel H U, Haase M 2004 Adv. Mater. 16 2102 Google Scholar
[12]	Mai H X, Zhang Y W, Sun L D, Yan C H 2007 J. Phys. Chem. C 111 13721 Google Scholar
[13]	Shi F, Wang J S, Zhai X S, Zhao D, Qin W P 2011 Cryst. Eng. Comm. 13 3782 Google Scholar
[14]	Yang T S, Sun Y, Liu Q, Feng W, Yang P Y, Li F Y 2012 Biomaterials 33 3733 Google Scholar
[15]	He E J, Zheng H R, Gao W, Tu Y X, Lu Y, Li G A 2013 Mater. Res. Bull. 48 3505 Google Scholar
[16]	Chang J, Liu Y, Li J, Wu S L, Niu W B, Zhang S F 2013 J. Mater. Chem. C 1 1168 Google Scholar
[17]	Gao D L, Zhang X Z, Zheng H R, Gao W, He E J 2013 J. Alloy. Compd. 554 395 Google Scholar
[18]	Gao W, Zheng H R, Han Q Y, He E J, Gao F Q, Wang R B 2014 J. Mater. Chem. C 2 5327 Google Scholar
[19]	何恩节, 郑海荣, 高伟, 鹿盈, 李俊娜, 魏映, 王灯, 朱刚强 2013 物理学报 62 237803 Google Scholar He E J, Zheng H R, Gao W, Lu Y, Li J N, Wei Y, Wang D, Zhu G Q 2013 Acta Phys. Sin. 62 237803 Google Scholar
[20]	Dong J, Gao W, Han Q Y, Wang Y K, Qi J X, Yan X W, Sun M T 2019 Rev. Phys. 4 100026 Google Scholar
[21]	Dong J, Zhang Z L, Zheng H R, Sun M T 2015 Nanophotonics 4 472
[22]	Li Y, Wang G F, Pan K, Fan N Y, Liu S, Feng L 2013 RSC Adv. 3 1683 Google Scholar
[23]	Rai M, Singh S K, Singh A K, Prasad R, Koch B, Mishra K, Rai S B 2015 ACS Appl. Mater. Inter. 7 15339 Google Scholar
[24]	Zuo J, Li Q Q, Xue B, Li C X, Chang Y L, Zhang Y L, Liu X M, Tu L P, Zhang H, Kong X G 2017 Nanoscale 9 7941 Google Scholar
[25]	Yi G S, Lu H C, Zhao S Y, Ge Y, Yang W J, Chen D P, Guo L H 2004 Nano Lett. 4 2191 Google Scholar
[26]	Chen X, Peng D, Ju Q, Wang F 2015 Chem. Soc. Rev. 44 1318 Google Scholar
[27]	Gao W, Dong J, Liu J H, Yan X W 2016 Mater. Res. Bull. 80 256 Google Scholar
[28]	高伟, 董军 2017 物理学报 66 204206 Google Scholar Gao W, Dong J 2017 Acta Phys. Sin. 66 204206 Google Scholar
[29]	Hu H, Chen Z G, Cao T Y, Zhang Q, Yu M G, Li F Y, Yi T, Huang C H 2008 Nanotechnology 19 375702 Google Scholar
[30]	Sangeetha N M, van Veggel F C J M 2009 J. Phys. Chem. C 113 14702 Google Scholar
[31]	Ye S, Chen G Y, Shao W, Junle Q, Paras N P 2015 Nanoscale 7 3976 Google Scholar
[32]	Xie X G, Ga N G, Deng R R, Sun Q, Xu Q H, Liu X G 2013 J. Am. Chem. Soc. 135 12608 Google Scholar
[33]	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
[34]	Vetrone B F, Naccache R, MahalingamV, Morgan C G, Capobianco J A 2009 Adv. Funct. Mater. 19 2924 Google Scholar
[35]	Gao W, Kong X Q, Han Q Y, Dong J, Zhang W W, Zhang B, Yan X W, Zhang Z L, He E J, Zheng H R 2018 J. Lumin. 196 186
[36]	Dong J, Zhang J, Han Q Y, Zhao X, Yan X W, Liu J H, Ge H B, Gao W 2019 J. Lumin. 207 361 Google Scholar

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[16]	Yang Jian-Zhi, Qiu Jian-Bei, Yang Zheng-Wen, Song Zhi-Guo, Yang Yong, Zhou Da-Cheng. Preparation and upconversion luminescence properties of Ba5SiO4Cl6: Yb3+, Er3+, Li+ phosphors. Acta Physica Sinica, 2015, 64(13): 138101. doi: 10.7498/aps.64.138101
[17]	Zheng Long-Jiang, Li Ya-Xin, Liu Hai-Long, Xu Wei, Zhang Zhi-Guo. Up-conversion luminescence and temperature characteristics of Tm3+, Yb3+ co-doped CaWO4 polycrystal material. Acta Physica Sinica, 2013, 62(24): 240701. doi: 10.7498/aps.62.240701
[18]	Zou Xiao-Cui, Wu Mu-Sheng, Liu Gang, Ouyang Chu-Ying, Xu Bo. First-principles study on the electronic structures of β-SiC/carbon nanotube core-shell structures. Acta Physica Sinica, 2013, 62(10): 107101. doi: 10.7498/aps.62.107101
[19]	Meng Qing-Yu, Chen Bao-Jiu, Zhao Xiao-Xia, Yan Bin, Wang Xiao-Jun, Xu Wu. Luminescence intensity of Ag+ doped Y2O3:Eu nanocrystals. Acta Physica Sinica, 2006, 55(5): 2623-2627. doi: 10.7498/aps.55.2623
[20]	Chen Xiao-Bo, Liu Kai, Zhang Jian, Wang Guo-Wen, Chen Chang-Tian. . Acta Physica Sinica, 2002, 51(3): 690-695. doi: 10.7498/aps.51.690

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Vol. 68, Issue 17 - 2019-09-05

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Enhanced red upconversion fluorescence emission of Ho³⁺ ions in NaLuF₄ nanocrystals through building core-shell structure

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

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Enhanced red upconversion fluorescence emission of Ho3+ ions in NaLuF4 nanocrystals through building core-shell structure

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

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Enhanced red upconversion fluorescence emission of Ho³⁺ ions in NaLuF₄ nanocrystals through building core-shell structure