Energy transfer characteristics of single-particle NaYF<sub>4</sub> core-shell structure

Gao Wei; Zhang Jing-Jing; Han Shan-Shan; Xing Yu; Shao Lin; Chen Bin-Hui; Han Qing-Yan; Yan Xue-Wen; Zhang Cheng-Yun; Dong Jun

doi:10.7498/aps.71.20221454

Abstract

The rare-earth doped micro/nano core-shell structure not only is beneficial to enhancing the upconversion emission intensity, but also can realize the fine control of luminescence color through the spatial separation of ions. In this work, a series of NaYF₄@NaYF₄ core-shell (CS) microcrystals doped with different ion concentrations is constructed by using the epitaxial growth technology. The structure and morphology for each of the prepared microcrystals are characterized by X-ray diffractometer (XRD) and scanning electron microscope (SEM). The experimental results show that the prepared CS structures each have a pure hexagonal-phase crystal structure, and exhibit a disk-like shape. Under the excitation of 980 nm laser, the energy transfer characteristics of doped ions in single CS microcrystal are carefully studied by using a confocal microscope spectroscopy test system and changing the excitation position. The study shows that the ions doped in different regions of the CS microdisks exhibit different spectral characteristics when the excitation position is changed, which is mainly due to the different directions of excitation energy transfer in the CS structure. Based on the emission spectra of different positions and power variation spectra, it is proved that the excitation energy of the micron CS is mainly transmitted from outside to inside. Meanwhile, the colorful emission pattern of the CS microdisk is revealed by the corresponding optical waveguide model, which is mainly due to the optical waveguide effect. Therefore, by constructing different micron core-shell structures, the luminescence characteristics of microcrystals can be controlled and adjusted, which can provide important experimental reference for the applications of microcrystals in optoelectronic devices, optical coding and multicolor display.

Keywords:

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. 12004304, 12104366 ), the Key R & D Program of Shaanxi Province, China (Grant No. 2022SF-333), the Shaanxi Provincial Research Plan for Young Scientific and Technological New Stars, China (Grant No. 2021KJXX-45), the Key Program of the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JZ-05), the Young Scientists Fund of the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JQ-041), and the Postgraduate Innovation Fund Project of Xi’an University of Posts and Telecommunications, China (Grant No. CXJJDL2021002).

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References

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Cited By

图 1 微/纳米晶体借助核壳结构实现上转换发射的模型示意图

Figure 1. Model schematic diagram of micro/nanocrystals up-conversion (UC) emission via core-shell (CS) structure.

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图 2 NaYF₄:20%Yb³⁺/2%Tm³⁺微米晶体及其包覆不同核壳结构的XRD图谱

Figure 2. The XRD patterns of NaYF₄:20%Yb³⁺ /2%Tm³⁺ microcrystals and their coating with different CS structures.

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图 3 NaYF₄:20%Yb³⁺/2%Tm³⁺微米晶体及包覆不同核壳结构的SEM及其相应的元素映射图　(a) NaYF₄:20%Yb³⁺/2%Tm³⁺; (b) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺; (c) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺@ NaYbF₄

Figure 3. The SEM images and element mappings of NaYF₄:20%Yb³⁺/2%Tm³⁺ microcrystals with corresponding CS structures: (a) NaYF₄:20%Yb³⁺/2%Tm³⁺; (b) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺; (c) NaYF₄:20%Yb³⁺/2%Tm³⁺ @ NaYF₄:20%Yb³⁺/2%Er³⁺@ NaYbF₄.

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图 4 共聚焦显微光谱测试系统示意图

Figure 4. Schematic diagram of the confocal microscope spectroscopic test system.

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图 5 在980 nm激发下, 单个NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺核壳微米盘在不同激发位置的　(a)上转换发射光谱(插图为不同激发位置下对应的发光照片), (b)蓝光、绿光和红光的发射峰面积, (c)增强倍数和(d)红绿比和红蓝比

Figure 5. (a) The UC emission spectra (The insert is corresponding optical micrographs at different excitation positions), (b) the peak area of the bule, green and red emission intensity, (c) enhancement and (d) R/G ratio and R/B ratio of the single NaYF₄:20%Yb³⁺/2%Tm³⁺@ NaYF₄:20%Yb³⁺/2%Er³⁺ CS microdisk at different excitation positions under the excitation of a 980 nm near-infrared (NIR) laser.

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图 6 在980 nm激发下, 单个NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄核-壳-壳微米盘在不同激发位置的　(a)上转换发射光谱(插图为不同激发位置下对应的发光照片), (b)蓝光、绿光和红光的发射峰面积, (c)增强倍数和(d)红绿比和红蓝比

Figure 6. (a) The UC emission spectra (The insert is corresponding optical micrographs at different excitation positions), (b) the peak area of the bule, green and red emission intensity, (c) enhancement and (d) R/G ratio and R/B ratio of the single NaYF₄:20%Yb³⁺/2%Tm³⁺@ NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄ core-shell-shell (CSS) microdisk at different excitation positions under the excitation of a 980 nm NIR laser.

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图 7 在980 nm激发下, 单个NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄核-壳-壳微米盘中Yb³⁺, Tm³⁺和Er³⁺离子在不同核壳体系之间所对应的能级图及跃迁机制图(插图为核-壳-壳微米盘的模型, 白点、绿点、蓝点和紫点分别代表Yb³⁺离子、Er³⁺离子、Tm³⁺离子和表面猝灭点)

Figure 7. The corresponding energy level diagrams and transition mechanism diagrams of Yb³⁺, Tm³⁺ and Er³⁺ ions between different CS systems in a single NaYF₄:20%Yb³⁺/2%Tm³⁺@ NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄ CSS microdisk under the excitation of a 980 nm NIR laser. (The inset is a model of a CSS microdisk, and the white, green, blue, and purple dots represent Yb³⁺ ions, Er³⁺ ions, Tm³⁺ ions, and surface quenching points, respectively.)

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图 8 在980 nm不同激发功率下, 单个(a) NaYF₄:20%Yb³⁺/2%Tm³⁺和(c) NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺微米盘在激发位置d的上转换发射光谱(插图为其对应的发光照片); (b), (d) 其蓝光, 绿光和红光发射强度与泵浦功率间的依赖关系

Figure 8. The UC emission spectra of a single (a) NaYF₄:20%Yb³⁺/2%Tm³⁺ and (c) NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺ microdisk at excitation position d under different excitation powers of a 980 nm NIR laser (The insert is corresponding optical micrographs); (b), (d) the dependence of its blue, green and red emission intensity on pump power.

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图 9 (a)—(d) 在980 nm激发下, 单个NaYF₄:Yb³⁺/Tm³⁺@NaYF₄:Yb³⁺/Er³⁺@NaYbF₄核-壳-壳微米盘分别在激发位置a, b, c, d的发光图案及其光波导模型

Figure 9. (a)–(d) The Luminescence patterns and optical waveguide models of a single NaYF₄:20%Yb³⁺/2%Tm³⁺@NaYF₄:20%Yb³⁺/2%Er³⁺@NaYbF₄ CSS microdisk at excitation positions a, b, c, d respectively under the excitation of a 980 nm NIR laser.

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表 1 水热法制备微米晶体的药品详细参数

Table 1. Detailed parameters of medicines for the preparation of microcrystals by hydrothermal method.

样品	核(核/壳)体积/mL	m(EDTA-2Na)/g	V(RE(NO₃)₃)/mL	V(NaF) /mL
NaYF₄:Yb³⁺/Tm³⁺	—	0.282	1.5	11.0
NaYF₄:Yb³⁺/Tm³⁺@NaYF₄:Yb³⁺/Er³⁺	5.0	0.282	1.5	11.0
NaYF₄:Yb³⁺/Tm³⁺@NaYF₄:Yb³⁺/Er³⁺@NaYbF₄	5.0	0.282	1.5	11.0
注: RE(NO₃)₃和NaF溶液均为0.5 mol/L水溶液.

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[1]	Gnach A, Bednarkiewicz A 2012 Nano Today 7 532 Google Scholar
[2]	Bettinelli M, Carlos L, Liu X G 2015 Phys. Today 68 38
[3]	Mandl G A, Cooper D R, Hirsch T, Seuntjens J, Capobianco J A 2019 Methods Appl. Fluoresc. 7 012004 Google Scholar
[4]	Zhang H X, Chen Z H, Liu X, Zhang F 2020 J. Nano Res. 13 1795 Google Scholar
[5]	Han Q Y, Zhao B C, Gao W, Li Y X, Sun Z Y, Wang C, Chen Y, Wang Y K, Yan X W, Dong J 2022 Phys. Chem. Chem. Phys. 24 13730 Google Scholar
[6]	Xiang Y, Zheng S S, Yuan S S, Wang J, Wu Y H, Zhu X H 2022 Mikrochim. Acta 189 120 Google Scholar
[7]	Li Y, Chen C, Liu F F, Liu J L 2022 Mikrochim. Acta 189 109 Google Scholar
[8]	Xu M M, Ge W Y, Zhang X M, Li Y X 2022 Opt. Laser Technol. 145 107529 Google Scholar
[9]	Alkahtani M, Almuqhim A A, Qasem H, Alsofyani N, Alfahd A, Alenzi S M, Aljuwayr A, Alzahrani Y A, Al-Badri A, Alotaibi M H, Bagabas A, AlHazaa A N, Hemmer P R 2021 Nanomaterials 11 2909 Google Scholar
[10]	Liu B T, Huang T H, Wang T L, Hsu C C 2021 Sol Energy 227 1 Google Scholar
[11]	Dong H, Sun L D, Yan C H 2021 J. Am. Chem. Soc. 143 20546 Google Scholar
[12]	Wang J, Sun X Y, Han Y D, Cheng Z Z, Liu T G 2021 Opt. Commun. 483 126663 Google Scholar
[13]	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 物理学报 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
[14]	Wang Y, Low J X, Bi Y F, Bai Y, Jiang Y W, Wang H H, Liu W Y, Ma Y Q, Chen Y N, Long R, Xiong Y J 2022 Chin. Chem. Lett. 33 1087 Google Scholar
[15]	Jia H, Li D G, Zhang D, Dong Y H, Ma S T, Zhou M, Di W H, Qin W P 2021 ACS Appl. Mater. Inter. 13 4402 Google Scholar
[16]	Chen T, Hao S W, Azimbay A, Shang Y F, Pi Q L, Hou Y D, Yang C H 2019 J. Power Sources 430 43 Google Scholar
[17]	Jiao X F, Ye W H, Huang Q Y, Luo G, Yu L L, Liu X T 2020 J. Rare Earths 38 697 Google Scholar
[18]	Ju D D, Gao X L, Zhang S C, Li Y, Cui W J, Yang Y H, Luo M Y, Liu S J 2021 CrystEngComm 23 3892 Google Scholar
[19]	Gao W, Sun Z Y, Han Q Y, Han S S, Cheng X T, Wang Y K, Yan X W, Dong J 2021 J. Alloys Compd. 857 157578 Google Scholar
[20]	Gao W, Zhang C X, Han Q Y, Lu Y R, Yan X W, Wang Y K, Yang Y, Liu J H, Dong J 2022 J. Lumin. 241 118501 Google Scholar
[21]	Felsted R G, Pant A, Bard A B, Xia X J, Luntz-Martin D R, Dadras S, Zhang S, Vamivakas A N, Pauzauskie P J 2022 Cryst. Growth Des. 22 3605 Google Scholar
[22]	Zhang Y H, Huang L, Liu X G 2016 Angew. Chem. Int. Ed. 55 5718 Google Scholar
[23]	He E J, Yu J J, Wang C, Jiang Y, Zuo X Z, Xu B, Wen J, Qin Y F, Wang Z J 2020 Mater Res Bull. 121 110613
[24]	Yang D D, Peng Z X, Zhan Q Q, Huang X J, Peng X Y, Guo X, Dong G P, Qiu J R 2019 Small 15 1904298 Google Scholar
[25]	Zhou Z Q, Xue J B, Zhang B P, Wang C, Yang X C, Fan W, Ying L Y, Zheng Z W, Xie Y J, Wu Y F, Yang X D, Zhang D 2021 Appl. Phys. Lett. 118 173301 Google Scholar
[26]	Mehrdel B, Nikbakht A, Aziz A A, Jameel M S, Dheyab M A, Khaniabadi P M 2022 Nanotechnology 33 082001 Google Scholar
[27]	Wu Y F S, Lai F Q, Liu B, Li Z B, Liang T X, Qiang Y C, Huang J H, Ye X Y, You W X 2020 J. Rare Earths 38 130 Google Scholar
[28]	Yan L, Zhou B, Song N, Liu X L, Huang J S, Wang T, Tao L L, Zhang Q Y 2018 Nanoscale 10 17949 Google Scholar
[29]	Wu Q X, Xu Z, Wageh S, Al-Ghamdia A, Zhao S L 2022 J. Alloys Compd. 891 162067 Google Scholar
[30]	赵越, 杨帆, 孙佳石, 李香萍, 张金苏, 张希珍, 徐赛, 程丽红, 陈宝玖 2019 物理学报 68 213301 Google Scholar Zhao Y, Yang F, Sun J S, Li X P, Zhang J S, Zhang X Z, Xu S, Cheng L H, Chen B J 2019 Acta Phys. Sin. 68 213301 Google Scholar
[31]	张翔宇, 王丹, 石焕文, 王晋国, 侯兆阳, 张力东, 高当丽 2018 物理学报 67 084203 Google Scholar Zhang X Y, Wang D, Shi H W, Wang J G, Hou Z Y, Zhang L D, Gao D L 2018 Acta Phys. Sin. 67 084203 Google Scholar
[32]	高伟, 孙泽煜, 郭立淳, 韩珊珊, 陈斌辉, 韩庆艳, 严学文, 王勇凯, 刘继红, 董军 2022 物理学报 71 034207 Google Scholar Gao W, Sun Z Y, Guo L C, Han S S, Chen B H, Han Q Y, Yan X W, Wang Y K, Liu J H, Dong J 2022 Acta Phys. Sin. 71 034207 Google Scholar
[33]	Kuang Y, Xu J T, Wang C, Li T Y, Gai S L, He F, Yang P P, Lin J 2019 Chem. Mater. 31 7898 Google Scholar
[34]	Gao W, Wang B Y, Han Q Y, Gao L, Wang Z J, Sun Z Y, Zhang B, Dong J 2020 J. Alloys Compd. 818 152934 Google Scholar
[35]	Gao D L, Wang D, Zhang X Y, Feng X J, Xin H, Yun S N, Tian D P 2018 J. Mater. Chem. C 6 622 Google Scholar

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Vol. 71, Issue 23 - 2022-12-05

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Energy transfer characteristics of single-particle NaYF₄ core-shell structure

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

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Energy transfer characteristics of single-particle NaYF4 core-shell structure

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

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Energy transfer characteristics of single-particle NaYF₄ core-shell structure