Tuning upconversion emissions of Ho<sup>3+</sup> through changing excitation conditions

Gao Wei; Wang Bo-Yang; Sun Ze-Yu; Gao Lu; Zhang Chen-Xue; Han Qing-Yan; Dong Jun

doi:10.7498/aps.69.20191333

Abstract

The upconversion (UC) emission properties of rare-earth ions are not only dependent on the host materials, but also relate to the excitation conditions. In this work, taking the Ho³⁺ ions for example, upconversion emission properties are studied in two NaYF₄ and LiYF₄ fluoride microcrystals through changing excitation conditions, namely the excitation power and the sample environment. The NaYF₄:20%Yb³⁺/2%Ho³⁺ and NaYF₄:20%Yb³⁺/2%Ho³⁺ microcrystal are synthesized by the hydrothermal method. The typical X-ray diffraction patterns of NaYF₄:20%Yb³⁺/2%Ho³⁺ and LiYF₄:20%Yb³⁺/2%Ho³⁺ microcrystal indicate that the prepared samples possess pure hexagonal phase NaYF₄ structure and the pure tetragonal phase LiYF₄ structure with high crystallinity, respectively. Most of NaYF₄:20%Yb³⁺/2%Ho³⁺ microcrystals show uniform and regular rod shape with diameter and length of approximately 3 μm and 10 μm, respectively. Few rods with a length of approximately 5 μm are also observed. The LiYF₄:20%Yb³⁺/2%Ho³⁺ microcrystals are all octahedral in shape with a smooth surface, the average size is around 10 μm. The spectral peculiarities of Ho³⁺ are investigated by using confocal microscopy equipment under near infrared 980 nm excitation. Beautiful patterns with different upconversion emissions of Ho³⁺ are discovered in single NaYF₄ and LiYF₄ microcrystal. As the excitation power increases, the upconversion emission of Ho³⁺ turns from green to pink in single NaYF₄ microrods due to the cross-relaxation between Ho³⁺ and the energy back transfer from Ho³⁺ to Yb³⁺. However, in single LiYF₄:Ho³⁺ microcrystal no similar phenomenon is observed. Nevertheless, when the powder of NaYF₄ and LiYF₄ microcrystals are excited by a 980 nm laser, increasing the power can turn the output colours of Ho³⁺ all green. Because particles outside the laser radiation are not directly covered by the laser, most of them are excited by the scattered light from the laser, and the actual excitation energy is low compared with at the center position. This result can be proved in the single NaYF₄ and LiYF₄ microcrystal under low excitation power. Thus, the results indicate that UC emission of rare-earth ions is controlled by changing the excitation condition. Using the new testing methods we can not only observe more interesting spectral phenomena, but also find a new way to further study its luminescence mechanism.

Keywords:

Authors and contacts

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

Corresponding author: Dong Jun, dongjun@xupt.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11604262), the Natural Science Basic Research Plan in Shaanxi Province, China (Grant No. 2018JM1052), the Shaanxi Provincial Research Plan for Young Scientific and Technological New Stars, China (Grant No. 2019KJXX-058), the International (Regional) Exchange Program of Shaanxi Province, China (Grant No. 2019KW-027), and the Research Plan of Xi’an University of Posts & Telecommunications, China (Grant No. CXJJ2017001)

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References

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图 1 (a) NaYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体和(b) LiYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体的XRD图谱

Figure 1. XRD patterns of (a) NaYF₄:20%Yb³⁺/2%Ho³⁺ and (b) LiYF₄:20%Yb³⁺/2%Ho³⁺ microcrystals.

DownLoad: Full-Size Img PowerPoint

图 2 (a) NaYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体和(b) LiYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体的SEM图谱

Figure 2. The SEM images of (a) NaYF₄:20%Yb³⁺/2%Ho³⁺ and (b) LiYF₄:20%Yb³⁺/2%Ho³⁺ microcrystals.

DownLoad: Full-Size Img PowerPoint

图 3 共聚焦显微光谱测试系统示意图

Figure 3. Schematic illustration of confocal microscopy setup.

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图 4 在980 nm激光激发下, 单颗NaYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体和LiYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体的上转换发射光谱图(激发功率为100 mW/cm²)

Figure 4. Upconversion emission spectra and corresponding optical micrographs of single NaYF₄:20%Yb³⁺/2%Ho³⁺ and LiYF₄:20%Yb³⁺/2%Ho³⁺ microcrystal under local excitation at 980 nm (100 mW/cm²).

DownLoad: Full-Size Img PowerPoint

图 5 在980 nm激光激发下, 单颗粒(a) NaYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体和(b) LiYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶的上转换发射与其激发功率的依赖关系, 插图为其对应光谱图案; (c)和(d)为对应不用激发功率下的峰面积, 插图为其随激发功率变化的红绿比图

Figure 5. (a), (b) Upconversion emission spectra and corresponding optical micrographs, (c), (d) the peak area of the green and red emission intensity and corresponding R/G ratio of single NaYF₄:20%Yb³⁺/2%Ho³⁺ (a), (c) and LiYF₄:20%Yb³⁺/2%Ho³⁺ (b), (d) microcrystal with excitation power densities increasing from 20 mW to 100 mW.

DownLoad: Full-Size Img PowerPoint

图 6 在980 nm激光激发下　(a) NaYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米粉末和(b) LiYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米粉末的上转换发射与其激发功率的依赖关系, 插图为其对应发光光谱图案; (c)和(d)为对应不用激发功率下的峰面积图, 插图为其随激发功率变化的红绿比图

Figure 6. (a), (b) UC emission spectra and corresponding optical micrographs, (c), (d) the peak area of the green and red emission intensity and corresponding R/G ratio of cluster NaYF₄:20%Yb³⁺/2%Ho³⁺ (a), (c) and LiYF₄:20%Yb³⁺/2%Ho³⁺ (b), (d) microcrystals with excitation power densities increasing from 20 mW to 100 mW.

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图 7 Ho³⁺离子相应的能级图及其可能跃迁机理图

Figure 7. Energy level diagrams and proposed energy transfer pathways.

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图 8 在532 nm激发下, 单粒NaYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶体和 LiYF₄:20.0%Yb³⁺/2.0%Ho³⁺微米晶的下转换发射光谱(a)及相应跃迁机理图(b)

Figure 8. (a) Downconversion emission spectra and (b) emission mechanism of single NaYF₄:20%Yb³⁺/2%Ho³⁺ and LiYF₄:20%Yb³⁺/2%Ho³⁺ microcrystal under laser 532 nm excitation.

DownLoad: Full-Size Img PowerPoint

[1]	Deng R, Qin F, Chen R, Huang W, Hong M, Liu X 2015 Nat. Nanotechnol. 10 237 Google Scholar
[2]	Sang J K, Zhou J Y, Zhang J C, Zhou H, Li H H, Ci Z P, Peng S L, Wang Z F 2019 ACS Appl. Mater. Interfaces 11 20150 Google Scholar
[3]	Wang Y H, Ohwaki J 1993 Appl. Phys. Lett. 63 3268 Google Scholar
[4]	Strassel K, Ramanandan S P, Abdolhosseinzadeh S, Diethelm M, Nuesch F, Hany R 2019 ACS Appl. Mater. Interfaces 11 23428 Google Scholar
[5]	Park Y I, Lee K T, Suh Y D, Hyeon T 2015 Chem. Soc. Rev. 44 1302 Google Scholar
[6]	Feng Y S, Wu Y N, Zuo J, Tu L P, Quec I, Chang Y L, Cruzc L J, Chanc A, Zhang H 2019 Biomaterials 201 33
[7]	Huang B L, Dong H, Wong K L, Sun L D, Yan C H 2016 J. Phys. Chem. C 120 18858 Google Scholar
[8]	Niu N, Yang P P, He F, Zhang X, Gai S L, Li C X, Lin J 2012 J. Mater. Chem. 22 10889 Google Scholar
[9]	Chen D Q, Yu Y L, Huang F, Yang A P, Wang Y S 2011 J. Mater. Chem. 21 6186 Google Scholar
[10]	Gao W, Wang R, Han Q, Dong J, Yan L, Zheng H 2015 J. Phys. Chem. C 119 2349
[11]	Huang P, Zheng W, Zhou S Y, Tu D T, Chen Z, Zhu H M, Li R F, Ma E, Huang M D, Chen X Y 2014 Angew. Chem. Int. Ed. 53 1252 Google Scholar
[12]	Zhou J J, Chen G X, Wu E, Bi G, Wu B T, Teng Y, Zhou S F, Qiu J R 2013 Nano Lett. 13 2241 Google Scholar
[13]	Ma C S, Xu X X, Wang F, Zhou Z G, Liu D M, Zhao J B, Guan M, Lang C I, Jin Y D 2017 Nano. Lett. 17 2858 Google Scholar
[14]	Han Q Y, Zhang C Y, Wang C, Wang Z J, Li C X, Gao W, Dong J, He E J, Zhang Z L, Zheng H R 2017 Sci. Rep. 7 5371 Google Scholar
[15]	Chen B, Kong W, Liu Y, Lu Y H, Li M Y, Qiao X S, Fan X P, Wang F 2017 Angew. Chem. Int. Ed. 56 10383 Google Scholar
[16]	Gao D L, Zhang X Y, Pang Q, Zhao J, Xiao G Q, Tian D 2018 J. Mater. Chem. C 6 8011 Google Scholar
[17]	Gao D L, Zhao D, Xin H, Cai A J, Zhang X Y 2019 J. Mater. Chem. C 7 11879 Google Scholar
[18]	Chen G Y, Liu H C, Somesfalean G, Liang H J, Zhang Z G 2009 Nanotechnology 20 385704 Google Scholar
[19]	Wu S J, Duan N, Li X L, Tan G L, Ma X Y, Xia Y, Wang Z P, Wang H X 2013 Talanta 116 611 Google Scholar
[20]	Tao F, Pan F, Wang Z J, Cai W L, Yao L Z 2010 CrystEngComm 12 4263 Google Scholar
[21]	高伟, 董军, 王瑞博, 王朝晋, 郑海荣 2016 物理学报 65 084205 Google Scholar Ga oW, Dong J, Wang R B, Wang Z J, Zheng H R 2016 Acta Phys. Sin. 65 084205 Google Scholar
[22]	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
[23]	Dominika P, Anna E, Bartosz F G, Tomasz G 2019 Sci. Rep. 9 8669 Google Scholar
[24]	Tan X J, Xu S L, Liu F H, Wang X Y, Goodman B A. Xiong D K, Deng W 2019 J. Lumin. 209 95 Google Scholar
[25]	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
[26]	Dai X, Lei L, Xia J, Han X, Hua Y, Xu S 2018 J. Alloys Compd. 766 261 Google Scholar
[27]	Schmidt T, Müller G, Spanhel L, Kerkel K, Forchel A 1998 Chem. Mater. 10 65 Google Scholar
[28]	Chen X P, Zhang Q Y, Yang C H, Chen D D, Zhao C 2009 Spectrochim. Acta., Part A 74 441 Google Scholar
[29]	Gao D L, Zhang X Y, Zheng H R, Gao W, He E J 2013 J. Alloys Compd. 554 395
[30]	Sangeetha N M, van Veggel F C J M 2009 J. Phys. Chem. C 113 14702 Google Scholar

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Tuning upconversion emissions of Ho³⁺ through changing excitation conditions

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Corresponding author: Dong Jun, dongjun@xupt.edu.cn

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Tuning upconversion emissions of Ho3+ through changing excitation conditions

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Corresponding author: Dong Jun, dongjun@xupt.edu.cn

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Tuning upconversion emissions of Ho³⁺ through changing excitation conditions