Upconversion white-light emission luminescence characteristics based on single-particle NaYF<sub>4 </sub>microrod

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

doi:10.7498/aps.72.20221606

Abstract

White upconversion (UC) luminescent materials have shown incomparable advantages over other light sources in the fields of solid-state lighting, liquid crystal display, and bioimaging, and received extensive attention from researchers. In this work, a series of microcrystals doped with different ion concentrations is synthesized by hydrothermal method, such as NaYF₄: Yb³⁺/Ho³⁺/Tm³⁺ and NaYF₄: Yb³⁺/Ho³⁺/Tm³⁺, and their corresponding micron core-shell (CS) structures are constructed based on epitaxial growth technology. The structure and morphology of the prepared microcrystals are characterised by X-ray diffractometer (XRD) and scanning electron microscope (SEM), showing that the microcrystal has a pure hexagonal-phase crystal structure with a rod-like shape. Under the excitation of 980 nm near-infrared laser, the white UC luminescence characteristics of Ho³⁺/Tm³⁺ and Er³⁺/Tm³⁺ co-doped single-particle NaYF₄ microcrystals are systematically studied by modulating the concentration of the doping ions. The study shows that in Ho³⁺/Tm³⁺ co-doped NaYF₄ microcrystals, white UC luminescence can be easily achieved by modulating the concentration of Yb³⁺ ions, while in the Er³⁺/Tm³⁺ co-doped NaYF₄ microcrystal, the white UC luminescence can be effectively achieved by modulating the concentration of Er³⁺ ions. According to the luminescence characteristics of the microncrystals in different doping systems, the physical mechanism of white light emission regulation is revealed, which is mainly due to the interaction between the doped ions, including cross relaxation (CR) process and energy back transfer (EBT) process. Meanwhile, an effective enhancement of the white UC luminescence on CS microrod is achieved by coating the NaYF₄ inert shell. Therefore, ion doping technique and the construction of CS structure can not only realize the white UC luminescence of microrods, but also provide important experimental reference for further enhancing the luminescence characteristics of microrods, and expand the applications of microcrystals in the fields of display, optoelectronics and anti-counterfeiting.

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: The project supported by the National Science Foundation of China (Grant Nos. 12004304, 12104366), the Key R & D Project of Shaanxi Province, China (Grant No. 2022SF-333), the Research Plan for Young Scientific and Technological New Stars of Shaanxi Province, China (Grant No. 2021KJXX-45), the Key Project of Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JZ-05), the Youth Project of Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JQ-041), and the Xi’an University of Posts and Telecommunications Joint Postgraduate Cultivation Workstation, China (Grant No. CXJJZL2021003).

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References

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[13]	Long S W, Ma D C, Zhu Y Z, Yang M M, Lin S P, Wang B 2017 J. Lumin. 192 728 Google Scholar
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Cited By

图 1 NaYF₄ : 9% Yb³⁺/ 2% Ho³⁺/2% Tm³⁺, NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺微米晶体及其核壳微米棒的XRD图谱

Figure 1. XRD patterns of NaYF₄ : 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺, NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺ microcrystals and their core-shell microrods.

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图 2 NaYF₄: 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺, NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺微米晶体及其核壳微米棒的(a1)—(a4) SEM图像, (b1)—(b4)元素映射图, (c1)—(c4)尺寸分布图

Figure 2. (a1)–(a4) SEM images, (b1)–(b4) element maps and (c1)–(c4) size distribution of NaYF₄: 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺ and NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺ microcrystals and their core-shell microcrystals.

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图 3 共聚焦显微光谱测试系统示意图

Figure 3. Schematic diagram of the confocal microscope spectroscopic test system.

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图 4 在980 nm激光激发下, 单颗粒NaYF₄ : x% Yb³⁺/2% Ho³⁺/2% Tm³⁺ (x = 6, 7, 8, 9)微米棒的(a)上转换发射光谱, (b)红光、绿光和蓝光的发射峰面积, (c)红绿比、蓝绿比和(d) CIE色度坐标图

Figure 4. (a) The UC emission spectra, (b) the peak area of the bule, green and red emission intensity, (c) R/G ratio, B/G ratio and (d) CIE chromaticity coordinates of single-particle NaYF₄ : x% Yb³⁺/2% Ho³⁺/2% Tm³⁺ (x = 6, 7, 8, 9) microrods under the excitation of 980 nm NIR laser.

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图 5 在980 nm激光激发下, 单颗粒NaYF₄ : 36% Yb³⁺/x% Er³⁺/2% Tm³⁺ (x = 0.5, 1.0, 1.5, 2.0)微米棒的(a)上转换发射光谱; (b)红光、绿光和蓝光的发射峰面积; (c)红绿比、蓝绿比以及(d) CIE色度坐标图

Figure 5. (a) The UC emission spectra, (b) the peak area of the bule, green and red emission intensity, (c) R/G ratio, B/G ratio and (d) CIE chromaticity coordinates of single-particle NaYF₄ : 36% Yb³⁺/x% Er³⁺/2% Tm³⁺ (x = 0.5, 1.0, 1.5, 2.0) microrods under the excitation of 980 nm NIR laser.

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图 6 在980 nm激光激发下, 单颗粒(a) NaYF₄ : 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺, (b) NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺微米棒及其惰性核壳结构的发射光谱, (c), (e)红光、绿光和蓝光的发射峰面积和(d), (f)增强倍数

Figure 6. (a)(b) The UC emission spectra, (c)(e) the peak area of the bule, green and red emission intensity and (d)(f) enhancement of single-particle NaYF₄ : 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺, NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺ and its inert core-shell microrods under the excitation of 980 nm NIR laser.

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图 7 在980 nm激光激发下, (a) NaYF₄ : Yb³⁺/Ho³⁺/Tm³⁺及(b) NaYF₄ : Yb³⁺/Er³⁺/Tm³⁺共掺体系的能量传递及其可能的跃迁机制图

Figure 7. Energy transfer and possible transition mechanism of (a) NaYF₄ : Yb³⁺/Ho³⁺/Tm³⁺ and (b) NaYF₄ : Yb³⁺/Er³⁺/Tm³⁺ co-doped systems under excitation of 980 nm NIR laser.

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图 8 在不同功率980 nm激光激发下, 单颗粒NaYF₄ : 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺及NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺微棒的(a)(d)发射光谱, (b)(e) 红光、绿光和蓝光的发射峰面积(插图为对应的R/G比值、B/G比值), 及(c)(f) 泵浦功率依赖关系

Figure 8. (a)(d) The UC emission spectra, (b)(e) the peak area of the bule, green and red emission intensity (insets show the corresponding R/G ratio, B/G ratio) and (c)(f) pump power dependences of single-particle NaYF₄ : 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺, NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺.

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图 A1 980 nm激光激发下, 单颗粒NaYF₄:x% Yb³⁺/2% Ho³⁺/2% Tm³⁺(x = 5, 10, 15, 18)微米棒的(a)上转换发射光谱, (b)红光、绿光、蓝光发射峰面积以及(c)红绿比、蓝绿比

Figure A1. (a) The UC emission spectra, (b) the peak area of the bule, green and red emission intensity, (c) R/G ratio, B/G ratio of single-particle NaYF₄: x% Yb³⁺/2% Ho³⁺/2% Tm³⁺ (x = 5, 10, 15, 18) microrods under the excitation of 980 nm NIR laser.

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图 A2 980 nm激光激发下, 单颗粒NaYF₄:x% Yb³⁺/2% Er³⁺/2% Tm³⁺(x = 10, 20, 30, 40, 45, 50)微米棒的(a)上转换发射光谱, (b)红光、绿光、蓝光发射峰面积以及(c)红绿比、蓝绿比

Figure A2. (a) The UC emission spectra, (b) the peak area of the bule, green and red emission intensity and (c) R/G ratio, B/G ratio of single-particle NaYF₄:x% Yb³⁺/2% Er³⁺/2% Tm³⁺(x = 10, 20, 30, 40, 45, 50) microrods under the excitation of 980 nm NIR laser.

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图 A3 980 nm激光激发下, 单颗粒NaYF₄:x% Yb³⁺/2% Er³⁺/2% Tm³⁺(x = 32, 34, 36, 38)微米棒的(a)上转换发射光谱, (b)红光、绿光、蓝光发射峰面积以及(c)红绿比、蓝绿比

Figure A3. (a) The UC emission spectra, (b) the peak area of the bule, green and red emission intensity and (c) R/G ratio, B/G ratio of single-particle NaYF₄:x% Yb³⁺/2% Er³⁺/2% Tm³⁺(x = 32, 34, 36, 38) microrods under the excitation of 980 nm NIR laser.

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表 1 水热法制备微米晶体所需药品的详细参数

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

样品	核体积/mL	EDTA-2Na/g	Re(NO₃)₃/mL	NaF/mL	NH₄HF₂/mL
NaYF₄:Yb³⁺/Ho³⁺/Tm³⁺	—	0.282	1.50	5.00	6.00
NaYF₄:Yb³⁺/Er³⁺/Tm³⁺	—	0.282	1.50	5.00	6.00
NaYF₄:Yb³⁺/Ho³⁺/Tm³⁺@NaYF₄	5	0.282	1.50	5.00	6.00
NaYF₄:Yb³⁺/Er³⁺/Tm³⁺@NaYF₄	5	0.282	1.50	5.00	6.00
注: Re(NO₃)₃, NaF和NH₄HF₂溶液浓度均为0.5 mol/L.

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表 2 单个NaYF₄ : x% Yb³⁺/2% Ho³⁺/2% Tm³⁺(x = 6, 7, 8, 9)微米棒的CIE色度坐标

Table 2. CIE coordinates of single-particle NaYF₄ : x% Yb³⁺/2% Ho³⁺/2% Tm³⁺(x = 6, 7, 8, 9) microrods.

Samples	CIE chromaticity coordinate
Samples	x	y
NaYF₄ : 6% Yb³⁺/2% Ho³⁺/2% Tm³⁺	0.3123	0.3824
NaYF₄ : 7% Yb³⁺/2% Ho³⁺/2% Tm³⁺	0.3215	0.3456
NaYF₄ : 8% Yb³⁺/2% Ho³⁺/2% Tm³⁺	0.3383	0.3932
NaYF₄ : 9% Yb³⁺/2% Ho³⁺/2% Tm³⁺	0.3284	0.3401

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表 3 单个NaYF₄ : 36% Yb³⁺/x% Er³⁺/2% Tm³⁺(x = 0.5, 1.0, 1.5, 2.0)微米棒的CIE色度坐标

Table 3. CIE coordinates of single-particle NaYF₄ : 36% Yb³⁺/x% Er³⁺/2% Tm³⁺(x = 0.5, 1.0, 1.5, 2.0) microrods.

Samples	CIE chromaticity coordinate
Samples	x	y
NaYF₄ : 36% Yb³⁺/0.5% Er³⁺/2% Tm³⁺	0.2604	0.3661
NaYF₄ : 36% Yb³⁺/1.0% Er³⁺/2% Tm³⁺	0.3281	0.3204
NaYF₄ : 36% Yb³⁺/1.5% Er³⁺/2% Tm³⁺	0.3216	0.3748
NaYF₄ : 36% Yb³⁺/2.0% Er³⁺/2% Tm³⁺	0.3018	0.4854

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[1]	Shao L, Liu D, Lyu J, Zhou D, Ding N, Sun R, Xu W, Wang N, Xu S, Dong B, Song H 2021 Mater. Today Phys. 21 100495 Google Scholar
[2]	Hao S, Shang Y F, Hou Y D, Chen T, Lv W Q, Hu P G, Yang C H 2021 Sol. Energy 224 563 Google Scholar
[3]	Liu H L, Xu J H, Wang H, Liu Y J, Ruan Q F, Wu Y M, Liu X G, Yang J K W 2019 Adv. Mater. 31 1807900 Google Scholar
[4]	Gao L X, Shan X C, Xu X X, Liu Y T, Liu B L, Li S Q, Wen S H, Ma C S, Jin D Y, Wang F 2020 Nanoscale 12 18595 Google Scholar
[5]	Liang H Z, Lei W C, Liu S X, Zhang P, Luo Z W, Lu A X 2021 Opt. Mater. 119 111320 Google Scholar
[6]	Du P, Bharat L K, Yu J S 2015 J. Alloys Compd. 633 37 Google Scholar
[7]	Ray S K, Joshi B, Ramani S, Park S, Hur J 2022 J. Alloys Compd. 892 162101 Google Scholar
[8]	Bao S, Yu H Y, Gao G Y, Zhu H Y, Wang D S, Zhu P F, Wang G F 2021 Nano Res. 15 3594
[9]	Li G G, Tian Y, Zhao Y, Lin J 2015 Chem. Soc. Rev. 44 8688 Google Scholar
[10]	Luitel H N, Chand R, Watari T 2016 Displays 42 1 Google Scholar
[11]	Vinodkumar P, Panda S, Jaiganesh G, Padhi R K, Madhusoodanan U, Panigrahi B S 2021 Spectrochim. Acta A Mol. Biomol. Spectrosc. 253 119560
[12]	Meng Z P, Zhang S F, Wu S L 2020 J. Lumin. 227 117566 Google Scholar
[13]	Long S W, Ma D C, Zhu Y Z, Yang M M, Lin S P, Wang B 2017 J. Lumin. 192 728 Google Scholar
[14]	Mehrdel B, Nikbakht A, Aziz A A, Jameel M S, Dheyab M A, Khaniabadi P M 2021 Nanotechnology 33 082001 Google Scholar
[15]	Shi F, Wang J S, Zhai X S, Zhao D, Qin W P 2011 CrystEngComm 13 3782 Google Scholar
[16]	Lin H, Xu D K, Teng D D, Yang S H, Zhang Y L 2015 Luminescence 30 723 Google Scholar
[17]	Pathak T K, Kumar A, Erasmus L J B, Pandey A, Coetsee E, Swart H C, Kroon R E 2018 Spectrochim. Acta A Mol. Biomol. Spectrosc. 207 23
[18]	Hassairi M A, Hernandez A G, Dammak M, Zambon D, Chadeyron G, Mahiou R 2018 J. Lumin. 203 707 Google Scholar
[19]	Xiao P, Ye S, Liao H Z, Shi Y L, Wang D P 2019 J. Solid State Chem. 275 63 Google Scholar
[20]	Ju D D, Song F, Han Y D, Zhang J, Song F F, Zhou A H, Huang W, Zadkov V 2019 J. Alloys Compd. 787 1120 Google Scholar
[21]	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
[22]	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
[23]	高伟, 王博扬, 孙泽煜, 高露, 张晨雪, 韩庆艳, 董军 2020 物理学报 69 034207 Google Scholar Gao W, Wang B Y, Sun Z Y, Gao L, Zhang C X, Han Q Y, Dong J 2020 Acta Phys. Sin. 69 034207 Google Scholar
[24]	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
[25]	Bao H Q, Wang W, Li X, et al. 2021 Adv. Opt. Mater. 10 2101702 Google Scholar
[26]	Tong L M, Lu E, Pichaandi J, Zhao G Y, Winnik M A 2016 J. Phys. Chem. C 120 6269 Google Scholar
[27]	Tang J F, Li G N, Yang C, Gou J, Luo D H, He H 2015 CrystEngComm 17 9048 Google Scholar
[28]	Sun J Y, Xue B, Du H Y 2013 Mat. Sci. Eng. B 178 822 Google Scholar
[29]	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
[30]	Zhang C M, Ma P A, Li C X, Li G G, Huang S S, Yang D M, Shang M M, Kang X J, Lin J 2011 J. Mater. Chem. 21 717 Google Scholar
[31]	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 Compds. 857 157578 Google Scholar
[32]	Kuang Y, Xu J, Wang C, Li T Y, Gai S L, He F, Yang P P, Lin J 2019 Chem. Mater. 31 7898 Google Scholar
[33]	Yu Z C, Zhou H F, Zhou G J, et al. 2017 Phys. Chem. Chem. Phys. 19 31675 Google Scholar
[34]	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
[35]	Wu Q X, Xu Z, Wageh S, Al-Ghamdia A, Zhao S L 2022 J. Alloys Compd. 891 162067 Google Scholar
[36]	Huo L L, Zhou J J, Wu R Z, Ren J F, Zhang S J, Zhang J J, Xu S Q 2016 Opt. Mater. Express 6 1056 Google Scholar
[37]	Pang T, Cao W H, Xing M M, Luo X X, Yang X F 2011 Opt. Mater. 33 485 Google Scholar
[38]	Gao D L, Zhang X Y, Chong B, Xiao G Q, Tian D P 2017 Phys. Chem. Chem. Phys. 19 4288 Google Scholar
[39]	Jeong S H, Kshetri Y K, Kim S H, Cho S H, Lee S W 2019 Prog. Nat. Sci. 29 549 Google Scholar
[40]	Pollnau M, Gamelin D R, Lüthi S R, Güdel H U 2000 Phys. Rev. B 61 3337 Google Scholar
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Vol. 72, Issue 2 - 2023-01-20

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Upconversion white-light emission luminescence characteristics based on single-particle NaYF₄microrod

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

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Upconversion white-light emission luminescence characteristics based on single-particle NaYF4 microrod

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

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Upconversion white-light emission luminescence characteristics based on single-particle NaYF₄microrod