Constructing micro/nano-photonics barcodes based on micro-region upconversion emission spectrum of single core-shell microcrystal

Gao Wei; Zhang Zheng-Yu; Zhang Jing-Lei; Ding Peng; Han Qing-Yan; Zhang Cheng-Yun; Yan Xue-Wen; Dong Jun

doi:10.7498/aps.73.20241015

Abstract

The construction of core-shell structures with different structural properties based on the epitaxial growth technique has become an effective technique for regulating the luminescence properties of micro/nanocrystals. In order to obtain richer spectral information, NaYF₄:50%Yb³⁺/2%Tm³⁺@NaYF₄@NaYF₄:20%Yb³⁺/2%Er³⁺@NaYF₄@NaYbF₄:2%Er³⁺ multilayered core-shell microcrystals are prepared by using multiple epitaxial growth through introducing surface modifiers and controlling their reaction conditions. The XRD and SEM results clearly show that the core-shell microcrystals possess a pure hexagonal crystal structure in the form of a disk. The microdesk has a thickness of about 2.32 μm and a diameter of about 28.31 μm. The upconversion luminescence characteristics of different single microcrystal structures are investigated by a confocal microspectroscopy system. In order to realize the selective excitation and emission of a single microcrystal, the spatial distribution of luminescent ions can be controlled through introducing an intermediate isolation layer. Under 980 nm laser excitation, different excitation sites of the single microdisk exhibit different upconversion emission characteristics. The significant blue (450 and 475 nm), red (648 nm) and green (524 and 540 nm) emissions are observed, which mainly originat from Tm³⁺ and Er³⁺ radiative transitions. Meanwhile, the red and blue upconversion emission intensities of the microcrystals are improved by using various shell layers. In addition, the luminescence and energy-transfer features of single microcrystals are explored by changing the excitation position. The experimental results demonstrate that the incorporation of NaYF₄ inert shells between luminescent layers can regulate luminescence and prevent ions from interacting. By utilizing the spectral fingerprint data of dopant ions in various shell layers, we create customizable micro-nano photonic barcodes and employ them for optical anti-counterfeiting detection. This study explores the use of constructed core-shell structures with luminescent tunable micron core-shell structures to acquire diverse spectral information and maintain stability through their structural properties. Thus, this core-shell structure provides a novel method for using upconversion luminescent microcrystals into micro- and nanophotonics to achieve anti-counterfeiting and display purposes.

Keywords:

Authors and contacts

School of Electronic Engineering, Xi’an University of Posts and 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 Natural Science Foundation of China (Grant No. 12274341), the Shaanxi Provincial Basic Science Research Project, China (Grant No. 23JSY007), the Key R & D Plan of Shaanxi Province, China (Grant No. 2023-YBGY-256), the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JZ-05), the Youth Program of the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JQ-041), the Education Department Service Local Special Program of Shaanxi Province, China (Grant No. 22JC-057), and the Xi’an University Talents Service Enterprise Project, China (Grant No. 23GXFW0089).

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References

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[9]	Zhou X Q, Ning L X, Qiao J W, Zhao Y F, Xiong P X, Xia Z G 2022 Nat. Commun. 13 7589 Google Scholar
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[11]	Chen J B, Li M S, Sun R R, Xie Y, Reimers J R, Sun L N 2024 Adv. Funct. Mater. 34 2315276 Google Scholar
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[17]	Gao W, Shao L, Han S S, Xing Y, Zhang J J, Chen B H, Han Q Y, Yan X W, Zhang C Y, Dong J 2023 Acta Phys. Sin. 72 024207 (in Chinses) [高伟, 邵琳, 韩珊珊, 邢宇, 张晶晶, 陈斌辉, 韩庆艳, 严学文, 张成云, 董军 2023 72 024207]Google Scholar Gao W, Shao L, Han S S, Xing Y, Zhang J J, Chen B H, Han Q Y, Yan X W, Zhang C Y, Dong J 2023 Acta Phys. Sin. 72 024207 (in Chinses)Google Scholar
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[24]	Sun J, Zhang Z H, Zhao H F, Jiang H 2016 Chin. J. Lumin. 37 526 (in Chinses) [苏俊, 张振华, 赵会峰, 姜宏 2016 发光学报 37 526]Google Scholar Sun J, Zhang Z H, Zhao H F, Jiang H 2016 Chin. J. Lumin. 37 526 (in Chinses)Google Scholar
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[26]	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
[27]	Bai X, Song H W, Pan G H, Lei Y Q, Wang T, Ren X G, Lu S Z, Dong B, Dai Q L, Fan L B 2007 J. Phys. Chem. C 111 13611 Google Scholar
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[31]	Lin H, Xu D K, Cheng Z Y, Li Y j, Xu L Q, Ma Y, Yang H S, Zhang Y L 2020 Appl. Surf. Sci. 514 146074 Google Scholar
[32]	Fan X M, Nie J H, Ying W T, Xu S Q, Gu J M, Liu S M 2021 Dalton Trans. 50 12234 Google Scholar
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Cited By

图 1 (a) NaYF₄:50%Yb³⁺/2%Tm³⁺及其包覆不同壳层后微米核壳晶体的XRD图谱; (b)—(f) 相应微米晶体及其核壳晶体的SEM图谱以及相应的元素映射图, 其中(b) NaYF₄:50%Yb³⁺/2%Tm³⁺; (c) Tm@Y; (d) Tm@Y@Er; (e) Tm@Y@Er@Y; (f) Tm@Y@Er@Y@Yb.

Figure 1. (a) XRD patterns of NaYF₄:50%Yb³⁺/2%Tm³⁺ with different core-shell microcrystals. (b)–(f) SEM images and element mapping of the NaYF₄:50%Yb³⁺/2%Tm³⁺ with different core-shell microcrystals: (b) NaYF₄:50%Yb³⁺/2%Tm³⁺; (c) Tm@Y; (d) Tm@Y@Er; (e) Tm@Y@Er@Y; (f) Tm@Y@Er@Y@Yb.

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图 2 在980 nm激光激发下, (a), (b) NaYF₄:50%Yb³⁺/2%Tm³⁺微米晶体包覆不同壳层阶段时不同激发位置处的上转换发射光谱, (c), (d) 发射峰面积及其红绿比与红蓝比. 插图为对应的发光图片; a, NaYF₄:50%Yb³⁺/2%Tm³⁺; b, Tm@Y; c, Tm@Y@Er; d, Tm@Y@Er@Y; e, Tm@Y@Er@Y@Yb

Figure 2. (a), (b) Upconversion emission spectra, (c), (d) emission peak areas and R/G ratio, R/B ratio NaYF₄:50%Yb³⁺/2%Tm³⁺ with different core-shell microcrystals under 980 nm laser excitation. The insert is corresponding luminescence micrographs. a, NaYF₄:50%Yb³⁺/2%Tm³⁺; b, Tm@Y; c, Tm@Y@Er; d, Tm@Y@Er@Y; e, Tm@Y@Er@Y@Yb.

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图 3 980 nm激光激发下, (a) 单颗粒Tm@Er@Yb及(b) 单颗粒Tm@Y@Er@Y@Yb微米核壳结构在不同激发位置处的上转换发射光谱(插图为其发光图片), 以及相应的(c) 强度变化图及(d) CIE图

Figure 3. Upconversion emission spectra of (a) Tm@Er@Yb and (b) Tm@Y@Er@Y@Yb core-shell microcrystals at different excitation conditions under 980 nm laser excitation (The insert is corresponding luminescence micrographs), and corresponding (c) emission peak area trends and (d) CIE coordinate chart.

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图 4 在980 nm激光激发下, 不同微米晶体粉体样品的(a)上转换发射光谱和(b)发射峰面积, 插图为其发光图片 (a, NaYF₄:50%Yb³⁺/2%Tm³⁺; b, Tm@Y; c, Tm@Y@Er; d, Tm@Y@Er@Y; e, Tm@Y@Er@Y@Yb)

Figure 4. (a) Upconversion emission spectra and (b) emission peak areas of the different powder samples under 980 nm laser excitation. The insert is corresponding luminescence micrograps. a, NaYF₄:50%Yb³⁺/2%Tm³⁺; b, Tm@Y; c, Tm@Y@Er; d, Tm@Y@Er@Y; e, Tm@Y@Er@Y@Yb.

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图 5 在980 nm激光激发下, Tm@Y@Er@Y@Yb核壳微米晶体不同激发位置, 单一NaYbF₄:2%Er³⁺, NaYF₄:20%Yb³⁺/2%Er³⁺, NaYF₄:50%Yb³⁺/2%Tm³⁺ 微米晶体在不同功率下的(a)—(f)上转换发射光及其(g)—(l)谱泵浦功率依赖性关系　(a), (g) NaYbF₄:2%Er³⁺壳; (b), (h) NaYF₄:20%Yb³⁺/2%Er³⁺壳; (c), (i) NaYF₄:50%Yb³⁺/2%Tm³⁺核; (d), (j) NaYbF₄:2%Er³⁺; (e), (k) NaYF₄:20%Yb³⁺/2%Er³⁺; (f), (l) NaYF₄:50%Yb³⁺/2%Tm³⁺

Figure 5. (a)–(f) Upconversion emission spectra and (g)–(l) pump power dependences of Tm@Y@Er@Y@Yb microcrystals at different excitation positions and NaYbF₄:2%Er³⁺, NaYF₄:20%Yb³⁺/2%Er³⁺, NaYF₄:50%Yb³⁺/2%Tm³⁺ microcrystals under 980 nm laser excitation at different powers: (a), (g) NaYbF₄:2%Er³⁺ shell; (b), (h) NaYF₄:20%Yb³⁺/2%Er³⁺ shell; (c), (i) NaYF₄:50%Yb³⁺/2%Tm³⁺ shell; (d), (j) NaYbF₄:2%Er³⁺; (e), (k) NaYF₄:20%Yb³⁺/2%Er³⁺; (f), (l) NaYF₄:50%Yb³⁺/2%Tm³⁺.

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图 6 在980 nm激光激发下, Tm@Y@Er@Y@Yb微米核壳中不同离子的能级图和可能的跃迁机制图

Figure 6. Under 980 nm excitation, energy level diagram and possible transition mechanism diagram in Tm@Y@Er@Y@Yb core-shell microcrystals

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图 7 (a) 光子条形码防伪概念验证; (b) 980 nm激光激发下, 不同激发位置处晶体的上转换发射光谱以及相应的光子学条形码; (c) 光子学条形码的组合及验证示意图

Figure 7. (a) Photonic barcoding proof-of-concept for anti-counterfeiting; (b) upconversion emission spectra of microcrystals and corresponding photonics barcodes under 980 nm laser excitation; (c) schematic illustration of photonics barcodes.

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map

[1]	Sun L D, Wang Y F, Yan C H 2014 Acc. Chem. Res. 47 1001 Google Scholar
[2]	Himmelstoß S F, Hirsch T 2019 Part. Part. Syst. Char. 36 1900235 Google Scholar
[3]	Hu Y, Yang Y M, Zhang X F, Wang X, Li X X, Li Y Q, Li T Y, Zhang H W 2020 J. Phys. Chem. C 124 24940 Google Scholar
[4]	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
[5]	Zhu X Y, Zhong H X, Zhang F 2023 Acc. Mater. Res. 4 536 Google Scholar
[6]	Zhang C Y, Yin Q X, Ge S K, Qi J X, Han Q Y, Gao W, Wang Y K, Zhang M D, Dong J 2024 Mater. Res. Bull. 176 112801 Google Scholar
[7]	Patnam H, Hussain S K, Yu J S 2023 Ceram. Int. 49 2967 Google Scholar
[8]	Ding M Y, Dong B, Lu Y, Yang X F, Yuan Y J, Bai W F, Wu S T, Ji Z G, Lu C H, Zhang K, Zeng H B 2020 Adv. Mater. 32 2002121 Google Scholar
[9]	Zhou X Q, Ning L X, Qiao J W, Zhao Y F, Xiong P X, Xia Z G 2022 Nat. Commun. 13 7589 Google Scholar
[10]	Yao Y N, Gao Z H, Lv Y C, Lin X Q, Liu Y Y, Du Y X, Hu F Q, Zhao Y S 2019 Angew. Chem. Int. Ed. 131 13941 Google Scholar
[11]	Chen J B, Li M S, Sun R R, Xie Y, Reimers J R, Sun L N 2024 Adv. Funct. Mater. 34 2315276 Google Scholar
[12]	Ying W T, Nie J H, Fan X M, Xu S Q, Gu J M, Liu S M 2021 Adv. Opt. Mater. 9 2100197 Google Scholar
[13]	Zheng B Z, Fan J Y, Chen B, Qin X, Wang J, Wang F, Deng R R, Liu X G 2022 Chem. Rev. 122 5519 Google Scholar
[14]	Fan Y, Liu L, Zhang F 2019 Nano Today 25 68 Google Scholar
[15]	Han Y D, Li H Y, Wang Y B, Pan Y, Huang L, Song F, Huang W 2017 Sci. Rep. 7 1320 Google Scholar
[16]	Gao W, Zhang J J, Han S S, Xing Y, Shao L, Chen B H, Han Q Y, Yan X W, Zhang C Y, Dong J 2022 Acta Phys. Sin. 71 234206 (in Chinses) [高伟, 张晶晶, 韩珊珊, 邢宇, 邵琳, 陈斌辉, 韩庆艳, 严学文, 张成云, 董军 2022 71 234206]Google Scholar Gao W, Zhang J J, Han S S, Xing Y, Shao L, Chen B H, Han Q Y, Yan X W, Zhang C Y, Dong J 2022 Acta Phys. Sin. 71 234206 (in Chinses)Google Scholar
[17]	Gao W, Shao L, Han S S, Xing Y, Zhang J J, Chen B H, Han Q Y, Yan X W, Zhang C Y, Dong J 2023 Acta Phys. Sin. 72 024207 (in Chinses) [高伟, 邵琳, 韩珊珊, 邢宇, 张晶晶, 陈斌辉, 韩庆艳, 严学文, 张成云, 董军 2023 72 024207]Google Scholar Gao W, Shao L, Han S S, Xing Y, Zhang J J, Chen B H, Han Q Y, Yan X W, Zhang C Y, Dong J 2023 Acta Phys. Sin. 72 024207 (in Chinses)Google Scholar
[18]	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 Google Scholar
[19]	Yang D D, Peng Z X, Guo X, Qiao S Q, Zhao P, Zhan Q Q, Qiu J R, Yang Z M, Dong G P 2021 Adv. Opt. Mater. 9 2100044 Google Scholar
[20]	Jin L M, Chen X, Siu C K, Wang F, Yu S F 2017 ACS Nano 11 843 Google Scholar
[21]	Zhou Z Q, Xue J B, Zhang B P, Wang C, Yang X C, Fan WF, 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
[22]	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 (in Chinses) [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 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 (in Chinses)Google Scholar
[23]	Wu W W, Chen D Q, Zhou Y, Wang Z Y, Ji Z G 2016 J. Alloys Compd. 682 275 Google Scholar
[24]	Sun J, Zhang Z H, Zhao H F, Jiang H 2016 Chin. J. Lumin. 37 526 (in Chinses) [苏俊, 张振华, 赵会峰, 姜宏 2016 发光学报 37 526]Google Scholar Sun J, Zhang Z H, Zhao H F, Jiang H 2016 Chin. J. Lumin. 37 526 (in Chinses)Google Scholar
[25]	Lüthi S R, Pollnau M, Güdel H U, Hehlen M P 1999 Phys. Rev. B 60 162 Google Scholar
[26]	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
[27]	Bai X, Song H W, Pan G H, Lei Y Q, Wang T, Ren X G, Lu S Z, Dong B, Dai Q L, Fan L B 2007 J. Phys. Chem. C 111 13611 Google Scholar
[28]	Mehrdel B, Nikbakht A, Aziz A A, Jameel M S, Dheyab M A, Khaniabadi P M 2022 Nanotechnology 33 082001 Google Scholar
[29]	Yan X W, Zhang J L, Zhang Z Y, Ding P, Han Q Y, Zhang C Y, Gao W, Dong J 2024 Acta Phys. Sin. 73 054206 (in Chinses) [严学文, 张景蕾, 张正宇, 丁鹏, 韩庆艳, 张成云, 高伟, 董军 2024 73 054206]Google Scholar Yan X W, Zhang J L, Zhang Z Y, Ding P, Han Q Y, Zhang C Y, Gao W, Dong J 2024 Acta Phys. Sin. 73 054206 (in Chinses)Google Scholar
[30]	Lee C, Park H, Kim W, Park S 2019 Phys. Chem. Chem. Phys. 21 24026 Google Scholar
[31]	Lin H, Xu D K, Cheng Z Y, Li Y j, Xu L Q, Ma Y, Yang H S, Zhang Y L 2020 Appl. Surf. Sci. 514 146074 Google Scholar
[32]	Fan X M, Nie J H, Ying W T, Xu S Q, Gu J M, Liu S M 2021 Dalton Trans. 50 12234 Google Scholar
[33]	Gao Z H, Yang S, Xu B Y, Zhang T J, Chen S W, Zhang W G, Sun X, Wang Z F, Wang X, Meng X G, Zhao Y S 2021 Angew. Chem. Int. Ed. 60 24519 Google Scholar

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Vol. 73, Issue 18 - 2024-09-20

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