Enhancing red upconversion emission of Ho3+ ions through constructing NaYF4:Yb3+/Ho3+/Ce3+@NaYF4:Yb3+/Nd3+ core-shell structures

Dong Jun; Zhang Chen-Xue; Cheng Xiao-Tong; Xing Yu; Han Qing-Yan; Yan Xue-Wen; Qi Jian-Xia; Liu Ji-Hong; Yang Yi; Gao Wei

doi:10.7498/aps.70.20210118

Abstract

The red upconversion (UC) emission of Ho³⁺ ions is located in an “optical window” range of the biological tissue, which has great prospects in the biology application. In this work, the NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:x%Yb³⁺ and NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/x%Nd³⁺ core-shell (CS) nanoparticles (NPs) are built based on the epitaxial growth technology by the high-temperature co-precipitation method in order to enhance red UC emission. The crystal structure and morphology of NaYF₄ CS NPs are characterized by X-ray diffraction and transmission electron microscope. It can be found that the morphology of NaYF₄ CS NPs changes from sphere into rod shape when coated with NaYF₄ shell, and has a pure hexagonal-phase crystal structure. Under 980 nm excitation, the red UC emission intensity of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:5%Yb³⁺ CS NPs is strongest and enhanced about 5.2 times than that of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺ NPs. Under 800 nm excitation, the red emission intensity of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺ CS NPs is increased about 6.1 times compared with that of the NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/5%Nd³⁺ CS NPs. This is because the constructed CS effectively reduces the non-radiative decay from the surface defects of NPs, and the doped Yb³⁺ and Nd³⁺ ions in the NaYF₄ shells can transfer more excitation energy to Ho³⁺ ions in the core. In addition, the NaYF₄: 20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺ CS NP is excited by dual-wavelengths co-excitation (800 nm + 980 nm). It is found that the red UC emission intensity under the co-excitation of dual-wavelengths is higher than the sum of the excitation intensities of two single wavelengths (800 nm and 980 nm), which is due to the synergistic effect generated under the co-excitation of 980 nm and 800 nm near infrared laser. Therefore, different CS structures constructed by introducing different energy transfer channels can achieve the enhancement of the red UC emission under different excitation conditions, and the dual-wavelength co-excitation provides a new way to improve the penetration depth and the detection sensitivity for further expanding the applications in the field of biomedicine.

Keywords:

Authors and contacts

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

Corresponding author: Gao Wei, gaowei@xupt.edu.cn

Funds: Project support by the Shaanxi Province International Cooperation and Exchange Program, China (Grant No. 2019KW-027), the Natural Science Basic Research Plan in Shaanxi Province of China (Grant No. 2019JQ-864), the Key R&D program of Shaanxi Province, China (Grant Nos. 2020GY-101, 2020GY-127), the Xi’an Science and Technology Innovation Talent Service Enterprise Project, China (Grant Nos. 2020KJRC0107, 2020KJRC0112), and the Funded by Xi’an University of Posts and Telecommunications Joint Postgraduate Cultivation Workstation, China (Grant No. YJGJ201905)

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References

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Cited By

图 1 NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺纳米晶体及相应核壳纳米晶体的XRD图

Figure 1. The XRD patterns of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺ nanoparticles (NPs) and core-shell (CS) structures.

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图 2 (a) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺纳米晶体、(b) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@ NaYF₄核壳纳米晶体、(c) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@ NaYF₄:15%Yb³⁺ 核壳纳米晶体和(d) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺ @NaYF₄:15% Yb³⁺/10%Nd³⁺核壳纳米晶体的TEM图, 插图分别为相应的粒径尺寸分布图

Figure 2. The TEM images and size distribution of the (a) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺ NPs, (b) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄ CS NPs, (c) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺ CS NPs, and (d) NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺ @NaYF₄:15%Yb³⁺/10%Nd³⁺ CS NPs.

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图 3 在近红外光980 nm激发下, NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺纳米晶体和NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:x %Yb³⁺ (x = 0, 5, 10, 15)核壳纳米晶体的(a)上转换发射光谱、(b)增强因子和(c)红绿比图

Figure 3. (a) Upconversion (UC) emission spectra, (b) enhancement factor and (c) R/G ratio of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺ NPs and NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:x %Yb³⁺ (x = 0, 5, 10, 15) CS NPs under the excitation of a 980 nm NIR laser.

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图 4 在近红外光800 nm激发下, NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/x %Nd³⁺ (x = 5, 10, 15, 20, 30, 40)核壳纳米晶体的(a)上转换发射光谱、(b)增强因子和(c)红绿比图

Figure 4. (a) The UC emission spectra, (b) enhancement factor and (c) R/G ratio of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/x %Nd³⁺ (x = 5, 10, 15, 20, 30, 40) CS NPs under the excitation of an 800 nm NIR laser.

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图 5 (a) 在980 nm近红外光激发下, NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:5%Yb³⁺核壳纳米晶体和(c)在800 nm近红外光激发下, NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺核壳纳米晶体的上转换发射光谱, 插图分别为其随激发功率变化的红绿比图; (b)和(d)为对应的发光强度与激发功率间的依赖关系

Figure 5. (a) and (c) The UC emission spectra and corresponding R/G ratio, (b) and (d) UC emission intensity versus excitation power of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:5%Yb³⁺ CS NPs with 980 nm excitation power increasing from 40 mW to 100 mW (a), (b) and NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺ CS NPs with 800 nm excitation power increasing from 70 mW to 130 mW (c), (d).

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图 6 Nd³⁺, Yb³⁺, Ho³⁺ 和 Ce³⁺离子的能级图和可能的上转换跃迁机理

Figure 6. Energy level diagrams of Nd³⁺, Yb³⁺, Ho³⁺ and Ce³⁺ ions as well as proposed UC mechanisms.

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图 7 在980 nm近红外光激发下, NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺纳米晶体和NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:x %Yb³⁺ (x = 0, 5, 10, 15) 核壳纳米晶体的上转换红光发射的寿命衰减曲线

Figure 7. Luminescence lifetimes of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺NPs and NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:x %Yb³⁺ (x = 0, 5, 10, 15) CS NPs under 980 nm excitation at 642 nm.

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图 8 分别在980 nm激发下、800 nm激发下、980 nm和800 nm共同激发下NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺核壳纳米晶体的(a)上转换发射光谱和(b)红绿比图

Figure 8. (a) The UC emission spectra and (b) R/G ratio of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺CS NPs under 980 nm, 800 nm and simultaneous 980 nm + 800 nm excitation.

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图 9 NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺核壳纳米晶体在(a) 不同980 nm激光功率下, 固定800 nm激光功率为120 mW时和(d) 不同800 nm激光功率下, 固定980 nm激光功率为120 mW时的上转换发射光谱; (b) 和 (e)为其对应的随不同波长激发功率变化的增强因子图; (c) 和 (f) 为其对应的随不同波长激发功率变化的红绿比图

Figure 9. (a), (d) The UC emission spectra, (b), (e) enhancement factor and (c), (f) R/G ratio of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺CS NPs on the excitation power of 980 nm with the power of 800 nm laser fixed at 120 mW ((a)–(c)) and NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺/20%Nd³⁺CS NPs on the excitation power of 800 nm with the power of 980 nm laser fixed at 120 mW ((d)–(f)).

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表 1 NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺纳米晶体和NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:x %Yb³⁺核壳纳米晶体的上转换红光发射的荧光寿命

Table 1. Luminescence lifetimes of NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺ NPs and NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:x %Yb³⁺ (x = 0, 5, 10, 15) CS NPs under 980 nm excitation at 642 nm.

Samples	Lifetime/μs
a: NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺	208.7 ± 4.7
b: NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄	555.4 ± 4.1
c: NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:5%Yb³⁺	667.6 ± 5.7
d: NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:10%Yb³⁺	499.8 ± 1.7
e: NaYF₄:20%Yb³⁺/2%Ho³⁺/12%Ce³⁺@NaYF₄:15%Yb³⁺	321.8 ± 1.3

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[4]	An M Y, Cui J B, He Q, Wang L Y 2013 J. Mater. Chem. B 1 1333 Google Scholar
[5]	Li J J, Cheng F F, Huang H P, Li L L, Zhu J J 2015 Chem. Soc. Rev. 44 7855 Google Scholar
[6]	Zhu Y R, Zhao S W, Zhou B, Zhu H, Wang Y F 2017 J. Phys. Chem. C 121 18909 Google Scholar
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[9]	Campos-Gonçalvesa I, Costa B F O, Santos R F, Durães L 2017 Mater. Design. 130 263 Google Scholar
[10]	Szczeszak A, Jurga N, Lis F 2020 Ceram. Int. 46 26382 Google Scholar
[11]	Rakov N, Maciel G S, Sundheimer M L, Menezes L D S, Gomes A S L, Messaddeq Y, Cassanjes F C, Poirier G, Ribeiro S J L 2002 J. Appl. Phys. 92 6337 Google Scholar
[12]	Liu Y F, Zhao J, Zhang Y, Zhang H F, Zhang Z L, Gao H P, Mao Y L 2019 J. Alloy. Compd. 810 151761 Google Scholar
[13]	Huang X Y, Lin J 2015 J. Mater. Chem. C 3 7652 Google Scholar
[14]	Zhan S P, Xiong J, Nie G Z, Wu S B, Hu J S, Wu X F, Hu S G, Zhang J, Gao Y Y, Liu Y X 2019 Adv. Mater. Interfaces 6 1802089 Google Scholar
[15]	Li X M, Zhang F, Zhao D Y 2015 Chem. Soc. Rev. 44 1346 Google Scholar
[16]	Nie Z Y, Ke X X, Li D N, Zhao Y L, Zhu L L, Qiao R, Zhang X L 2019 J. Phys. Chem. C 123 22959 Google Scholar
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[19]	Shi Z L, Duan Y, Zhu X J, Wang Q W, Li D D, Hu K, Feng W, Li F Y, Xu C X 2018 Nanotechnology 29 094001 Google Scholar
[20]	Xu B, Zhang X, Huang W J, Yang Y J, Ma Y, Gu Z J, Zhai T Y, Zhao Y L 2016 J. Mater. Chem. B 4 2776 Google Scholar
[21]	Cui X S, Cheng Y, Lin H, Wu Q P, Xu J, Wang Y S 2019 J. Rare Earth. 37 573 Google Scholar
[22]	Vetrone F, Boyer J C, Capobianco J A, Speghini A, Bettinelli M 2004 J. Appl. Phys. 96 661 Google Scholar
[23]	Tian G, Gu Z J, Zhou L J, Yin W Y, Liu X X, Yan L, Jin S, Ren W L, Xing G M, Li S J, Zhao Y L 2012 Adv. Mater. 24 1226 Google Scholar
[24]	Li Y, Wang G F, Pan K, Fan N Y, Liu S, Feng L 2013 RSC Adv. 3 1683 Google Scholar
[25]	Gao W, Kong X Q, Han Q Y, Chen Y, Zhang J, Zhao X, Yan X W, Liu J H, Shi J, Dong J 2018 J. Lumin. 202 381 Google Scholar
[26]	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 Z 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
[27]	Gao W, Dong J, Liu J H, Yan X W 2016 J. Lumin. 179 562 Google Scholar
[28]	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
[29]	Gao W, Dong J, Yan X W, Liu L, Liu J H, Zhang W W 2017 J. Lumin. 192 513 Google Scholar
[30]	Gao W, Wang B Y, Han Q Y, Gao L, Wang Z J, Sun Z Y, Zhang B, Dong J 2020 J. Alloy. Compd. 818 152934 Google Scholar
[31]	Chen D Q, Liu L, Huang P, Ding M Y, Zhong J S, Ji Z G 2015 J. Phys. Chem. Lett. 6 2833 Google Scholar
[32]	Li J C, Zhu X J, Xue M, Feng W, Ma R L, Li F Y 2016 Inorg. Chem. 55 10278 Google Scholar
[33]	Vetrone F, Naccache R, Mahalingam V, Morgan C G, Capobianco J A 2009 Adv. Funct. Mater. 19 2924 Google Scholar
[34]	Kuang Y, Xu J T, Wang C, Li T Y, Gai S L, He F, Yang P P 2019 Chem. Mater. 31 7898 Google Scholar
[35]	Zhao J, Liu Y F, Zhou C P, Gao H P, Zhang H F, Mao Y L 2020 J. Lumin. 219 116936 Google Scholar
[36]	Gao D L, Zhang X Y, Chong B, Xiao G Q, Tian D P 2017 Phys. Chem. Chem. Phys. 19 4288 Google Scholar
[37]	Wang J M, Lin H, Cheng Y, Cui X S, Gao Y, Ji Z L, Xu J, Wang Y S 2019 Sensor Actuat. B-Chem. 278 165 Google Scholar
[38]	Chen Z, Zhang X W, Zeng S F, Liu Z J, Ma Z J, Dong G P, Zhou S F, Liu X F, Qiu J R 2015 Applied Physics Express 8 032301 Google Scholar
[39]	Zhou J J, Deng J Y, Zhu H M, Chen X Y, Teng Y, Jia H, Xu S Q, Qiu J R 2013 J. Mater. Chem. C 1 8023 Google Scholar
[40]	Yang Y, Li W W, Mei B C, Song J H, Yi G Q, Zhou Z W, Liu J S 2019 J. Lumin. 213 504 Google Scholar
[41]	Li P, Guo L N, Zhang Z X, Li T S, Chen P L 2018 Dyes and Pigments 154 242 Google Scholar

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Vol. 70, Issue 15 - 2021-08-05

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Enhancing red upconversion emission of Ho³⁺ ions through constructing NaYF₄:Yb³⁺/Ho³⁺/Ce³⁺@NaYF₄:Yb³⁺/Nd³⁺ core-shell structures

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Corresponding author: Gao Wei, gaowei@xupt.edu.cn

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