Red upconversion emission of Er3+ enhanced by building NaErF4@ NaYbF4:2%Er3+ core-shell structure

Gao Wei; Luo Yi-Fan; Xing Yu; Ding Peng; Chen Bin-Hui; Han Qing-Yan; Yan Xue-Wen; Zhang Cheng-Yun; Dong Jun

doi:10.7498/aps.72.20230762

Abstract

Building core-shell structures are widely used to enhance and regulate the luminescence properties of rare-earth-doped micro/nano materials. In this work, a variety of different NaErF₄ core-shell and core-shell-shell nanocrystals are successfully constructed based on high temperature co-precipitation method by epitaxial growth technology. The upconversion red emission intensities of Er³⁺ ions in different core-shell structures are effectively enhanced by regulating their structures and doping ions. The experimental structures show that the constructed core-shell nanocrystals each have a hexagonal phase structure, and core-shell structure of about 40 nm. In the near infrared 980 nm laser excitation, the NaErF₄ core-shell nanocrystal shows a strong single-band red emission. And the single-band red emission intensity of Er³⁺ ions is enhanced through constructing the NaErF₄@NaYbF₄:2%Er³⁺ core-shell structure. The experimental results show that red emission intensity of Er³⁺ ions is about 1.4 times higher than that of the NaErF₄@NaYbF₄ core-shell structure by constructing the NaErF₄@NaYbF₄:2%Er³⁺ core-shell structures under 980 nm excitation, and its red/green emission intensity ratio increases from 5.4 to 6.5. Meanwhile, when NaErF₄@NaYbF₄:2%Er³⁺ core-shell structure recoats the NaYF₄ inert shell and is added with a small quantity of Tm³⁺ ions, their red emission intensities of Er³⁺ ions are 23.2 times and 40.3 times that of NaErF₄@NaYbF₄ core-shell structures, and their red/green emission intensity ratios reach 7.5 and 10.2, respectively. The red emission enhancement of Er³⁺ ions is mainly caused by bidirectional energy transfer process of high excitation energy of Yb³⁺ ions and energy trapping center of Tm³⁺ ions which effectively change the density of population of luminescent energy levels of Er³⁺ ions. Furthermore, the coated NaYF₄ inert shell also effectively weakens the surface quenching effect of nanocrystals. The mechanisms of red enhancement in different core-shell structures are discussed based on the spectral properties, the process of interion energy transfer, and luminescence kinetics. The constructed NaErF₄@NaYbF₄:2%Er³⁺@NaYF₄ core-shell structures with high-efficiency red emission in this work have great potential applications in the fields of colorful anti-counterfeiting, display and biological imaging.

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. 12274341, 12004304, 12104366 ), the Key R & D Plan Program of Shaanxi Province, China (Grant No. 2022SF-333), the Natural Science Foundation of Shaanxi Province, China (Grant No. 2022JZ-05), the Natural Science Foundation Youth Program of Shaanxi Province, China (Grant No. 2022JQ-041), the Education Department Service Local Special Program of Shaanxi Province, China (Grant No. 22JC057), and the Innovation Fund Project of Xi’an University of Posts and Telecommunications, China (Grant No. CXJJY2022033).

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References

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Cited By

图 1 NaErF₄@NaYbF₄及其包覆不同核壳结构的XRD图谱

Figure 1. The XRD patterns of NaErF₄@NaYbF₄ and different C-S structures.

DownLoad: Full-Size Img PowerPoint

图 2 NaErF₄@NaYbF₄及其包覆不同核壳结构的TEM和粒径分布

Figure 2. The TEM images and size distribution of NaErF₄@NaYbF₄ and different C-S structures.

DownLoad: Full-Size Img PowerPoint

图 3 在980 nm激发下, NaErF₄@NaYbF₄及其包覆不同核壳结构的(a)上转换发射光谱, (b)红绿比和(c)红、绿发射光积分强度

Figure 3. (a) The UC emission spectra, (b) R/G ratio (c) red and green emission integration intensity of NaErF₄@NaYbF₄ and their coating with different C-S structures under 980 nm excitation.

DownLoad: Full-Size Img PowerPoint

图 4 在980 nm不同激发功率下　(a)NaErF₄:0.5%Tm³⁺@NaYbF₄:2%Er³⁺@NaYF₄ C-S晶体的上转换发射光谱; (b)红、绿光发射与泵浦功率依赖关系; (c)红、绿光发射强度对比(插图为其对应的红绿比)

Figure 4. (a) The UC emission spectra , (b) power density dependence of red and green emission, and (c) comparison of red and green emission intensity of NaErF₄:0.5%Tm³⁺@NaYbF₄:2%Er³⁺ @ NaYF₄ C-S structure under different excitation powers of 980 nm (The insert is corresponding R/G ratio).

DownLoad: Full-Size Img PowerPoint

图 5 在980 nm激光激发下, NaErF₄@NaYbF₄及其包覆的不同核壳结构所对应的能级图及可能的跃迁机理图

Figure 5. The corresponding energy level diagrams and possible transition mechanism diagrams of NaErF₄@ NaYbF₄ and their coating with different C-S structures under 980 nm excitation.

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图 6 在980 nm脉冲激光激发下, NaErF₄@NaYbF₄及其包覆不同核壳结构的寿命衰减曲线图

Figure 6. The decay curves of NaErF₄@NaYbF₄ and their coating with different C-S structures under the excitation of a 980 nm pulse laser.

DownLoad: Full-Size Img PowerPoint

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[2]	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
[3]	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
[4]	Wang Y B, Lei L, Ye R G, Jia G H, Hua Y J, Deng D G, Xu S Q 2021 ACS Appl. Mater. Interfaces 13 23951 Google Scholar
[5]	Bao H Q, Wang W, Li X, Liu X M, Zhang L, Yan X, Wang Y H, Wang C G, Jia X T, Sun P, Kong X G, Zhnag H, Lu G Y 2022 Adv. Optical Mater. 10 2101702 Google Scholar
[6]	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 物理学报 68 174204 Google Scholar Yan X W, Wang C 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
[7]	Meng Z P, Zhang S F, Wu S L 2020 J. Lumin. 227 117566 Google Scholar
[8]	Tang M, Zhu X H, Zhang Y H, Zhang Z P, Zhang Z M, Mei Q S, Zhang J, Wu M H, Liu J L, Zhang Y 2019 ACS Nano 13 10405 Google Scholar
[9]	Wang W, Feng Z, Li B, Chang Y L, Li X, Yan X, Chen R Z, Yu X M, Zhao H Y, Lu G Y, Kong X G, Qian J, Liu X M 2021 J. Mater. Chem. B 9 2899 Google Scholar
[10]	Xu F, Sun Y, Gao H P, Jin S Y, Zhang Z L, Zhang H F, Pan G C, Kang M, Ma X Q, Mao Y L 2021 ACS Appl. Mater. Interfaces 13 2674 Google Scholar
[11]	Tan M L, Li F, Wang X, Fan R W, Chen G Y 2020 ACS Nano 14 6532 Google Scholar
[12]	Zhang H B, Chen Z H, He Y R, Yang S Y, Wei J 2021 ACS Appl. Mater. Interfaces 4 4340
[13]	Lin H, Xu D K, Li A M, Teng D D, Yang S H, Zhang Y L 2016 Sci. Rep. 6 28051 Google Scholar
[14]	Lin H, Xu D K, Li A M, Qiu Z R, Yang S H, Zhang Y L 2017 New J. Chem. 41 1193 Google Scholar
[15]	Seki K, Uematsu K, Toda K, Sato M 2014 Chem. Lett. 43 1213 Google Scholar
[16]	Lin H, Xu D K, Li Y J, Yao L, Xu L Q, Ma Y, Yang S H, Zhang Y L 2018 Inorg. Chem. 57 15361 Google Scholar
[17]	Joshi R, Perala R S, Shelar S B, Ballal A, Singh B P, Ningthoujam S 2021 ACS Appl. Mater. Interfaces 13 3481 Google Scholar
[18]	Cheng Q, Sui J H, Cai W 2012 Nanoscale 4 779 Google Scholar
[19]	Lin H, Cheng Z Y, Xu D K, Zhang X G, Ge J, Xu L Q, Ma Y, Yang S H, Zhang Y L 2021 J. Mater. Chem. C 9 4385 Google Scholar
[20]	Lin H, Xu D K, Cheng Z Y, Li Y G, Xu L Q, Ma Y, Yang S H, Zhang Y L 2020 Appl. Surf. Sci. 514 146074 Google Scholar
[21]	Ren P, Zheng X L, Zhang J, Camillis S D, Jia J G, Wang H, Liao X Z, Piper J A, Lu Y Q 2022 ACS Photonics 9 758
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[24]	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. Interfaces 13 4402 Google Scholar
[25]	Shang Y F, Hao S W, Lv W Q, Chen T, Tian L, Lei Z T, Yang C H 2018 J. Mater. Chem. C 6 3869 Google Scholar
[26]	Choi J E, Kim D, Jang H S 2019 Chem. Commun. 55 2261 Google Scholar
[27]	Huang J S, Yan L, Liu S B, Song N, Zhang Q Y, Zhou B 2021 Adv. Funct. Mater. 31 2009796 Google Scholar
[28]	Xie X Y, Li Q Q, Chen H R, Wang W, Wu F X, Tu L P, Zhang Y L, Kong X G, Chang Y L 2022 Nano Lett. 22 5339 Google Scholar
[29]	Li D, Wen S H, Kong M Y, Liu Y T, Hu W, Shi B Y, Shi X Y, Jin D Y 2020 Anal. Chem. 92 10913 Google Scholar
[30]	Szczeszak A, Jurga N, Lis S 2020 Ceram. Int. 46 26382 Google Scholar
[31]	Tong L M, Lu E, Pichaandi J, Zhao G Y, Winnik M A 2016 J. Phys. Chem. C 120 6269 Google Scholar
[32]	Chen Q S, Xie X J, Huang B L, Liang L L, Han S Y, Yi Z G, Wang Y, Li Y, Fan D Y, Huang L, Liu X G 2017 Angew. Chem. Int. Ed. 56 7605 Google Scholar
[33]	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
[34]	Cui X S, Cheng Y, Lin H, Wu Q P, Xu J, Wang Y S 2019 J. Rare Earths 37 573 Google Scholar
[35]	Qiao Y F, Qiao S Q, Yu X, Min Q H, Pi C J, Qiu J B, Ma H Q, Yi J H, Zhan Q Q, Xu X H 2021 Nanoscale 13 8181 Google Scholar
[36]	Gao W, Xing Y, Chen B H, Shao L, Zhang J J, Yan X W, Han Q Y, Zhang C Y, Liu L, Dong J 2023 J. Alloys Compd. 936 168371 Google Scholar
[37]	Wu Q X, Xu Z, Wageh S, Al-Ghamdi A, Zhao S L 2021 J. Alloys Compd. 891 162067
[38]	Yan L, Huang J S, An Z C, Zhang Q Y, Zhou B 2022 Nano Lett. 22 7042 Google Scholar
[39]	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
[40]	Gao D L, Zhang X Y, Chong B, Xiao G Q, Tian D P 2017 Phys. Chem. Chem. Phys. 19 4288 Google Scholar
[41]	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

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Vol. 72, Issue 17 - 2023-09-05

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Red upconversion emission of Er³⁺ enhanced by building NaErF₄@ NaYbF₄:2%Er³⁺ core-shell structure