Synthesis and luminescent properties of rare earths doped Gd2Te4O11 tellurite phosphors

Luo Jie; Zhang Zi-Qiu; Xu Jun-Hao; Qin Zhao-Ting; Zhao Yuan-Shuai; He Hong; Li Guan-Nan; Tang Jian-Feng

doi:10.7498/aps.72.20221341

Abstract

A series of rare earth Dy³⁺, Tb³⁺, Eu³⁺ singly doped Gd₂Te₄O₁₁ (GTO) tellurite phosphors with intrinsic polarity are prepared by hydrothermal method. The phase structures, morphologies and thermal stabilities of these phosphors are characterized. Their luminescence properties are tested in detail. The results show that all those phosphors are crystalized into single phase of digadolinium tellurite with short rod-like shape. The maximum size in the axial direction is microns. The phosphor has good thermal stability. For the GTO:Dy³⁺, the fluorescence emission under UV excitation is mainly located in the yellow-green region. The optimal doping concentration corresponding to the strongest excitation and emission is 2.5%, and the CIE color coordinates are (0.39, 0.43). The fluorescence decay curve shows that the lifetime of the GTO:Dy³⁺ on ⁴F_9/2 energy level decreases gradually with doping concentration of Dy³⁺ increasing, which may be related to the cross relaxation (CR) between Dy³⁺ ions. For the GTO:Eu³⁺, the fluorescence emission under UV excitation is mainly located in the red region and orange-red region. The emission intensity is enhanced with the doping concentration of Eu³⁺ increasing. When the doping concentration is 10%, the CIE color coordinates are (0.62, 0.38), which are located in the orange-red region with high color purity. The fluorescence lifetime of Eu³⁺ on ⁵D₀ energy level is hardly affected by the change of Eu³⁺ doping concentration. For the GTO:Tb³⁺, with the increase of the Tb³⁺ concentration, the fluorescence emission under UV excitation changes from blue-violet region to yellow-green region, which can be ascribed to the influence of CR between Tb³⁺ ions. The fluorescence decay behavior reveals that the Tb³⁺ ions on ⁵D₄ excited state may undergo energy transfer and reabsorption, which can deviate the fluorescence decay from the single exponential model. When the concentration of Tb³⁺ is 0.5%, the sample exhibits white light emission with the CIE color coordinates of (0.33, 0.35) and color rendering index of 86. The measurements of temperature-dependent emission spectra show that the above-mentioned phosphors have good luminescent thermal stability. The internal quantum efficiencies (IQEs) of those three types of phosphors are measured, and the IQE of GTO:Eu³⁺ is better than those of GTO:Dy³⁺ and GTO:Tb³⁺. There is still much room for improvement in the luminescent performance of all these phosphors. These phosphors have potential to be used in UV-excited white LEDs.

Keywords:

Authors and contacts

School of Materials and Energy, Southwest University, Chongqing 400715, China

Corresponding author: Tang Jian-Feng, tangjf@swu.edu.cn

Funds: Project supported by the Natural Science Foundation of Chongqing, China (Grant No. cstc2020jcyj-msxmX0142) and the Innovation Program of Chongqing for Returnees (Grant No. cx2020102).

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References

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[2]	Fang M H, Bao Z, Huang W T, Liu R S 2022 Chem. Rev. 122 11474 Google Scholar
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[4]	Zhang X H, Lu Z M, Meng F B, Hu L, Xu X W, Lin J, Tang C C 2012 Mater. Lett. 79 292 Google Scholar
[5]	Yu X F, Yuan D W, Mi X Y 2021 J. Alloys Compd. 857 157585 Google Scholar
[6]	余阳, 刘自军, 陈乔乔, 戴能利, 李进延, 杨旅云 2013 物理学报 62 017804 Google Scholar Yu Y, Liu Z J, Chen Q Q, Dai N L, Li J Y, Yang L Y 2013 Acta Phys. Sin. 62 017804 Google Scholar
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[8]	Christy A G, Mills S J, Kampf A R 2016 Mineral. Mag. 80 415 Google Scholar
[9]	Shannon R D 1976 Acta Crystallogr. 32 751 Google Scholar
[10]	Zhang Z Q, Qin Z T, Zeng L W, Liu J, Li G N, Li C M, Yang J, Capobianco J A, Tang J F 2022 Ceram. Int. 48 13960 Google Scholar
[11]	You P L, Yin G F, Chen X C, Yue B, Huang Z B, Liao X M, Yao Y D 2011 Opt. Mater. 33 1808 Google Scholar
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[15]	Gupta S K, Zuniga J P, Abdou M, Thomas M P, Goonatilleke M D A, Guiton B S, Mao Y B 2020 Chem. Eng. J. 379 122314 Google Scholar
[16]	Li W L, Chen Z Y, Zhang B, Zhao P J, Fan Y W 2022 J. Lumin. 246 118824 Google Scholar
[17]	Yu R J, Shin D S, Jang K W, Guo Y, Noh H M, Moon B K, Choi B C, Jeong J H, Yi S S 2014 Spectrochim. Acta A Mol. Biomol. 125 458 Google Scholar
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[19]	赵旺, 平兆艳, 郑庆华, 周薇薇 2018 物理学报 67 247801 Google Scholar Zhao W, Ping Z Y, Zheng Q H, Zhou W W 2018 Acta Phys. Sin. 67 247801 Google Scholar
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[25]	Wu Y F, Nien Y T, Wang Y J, Chen I G 2012 J. Am. Ceram. Soc. 95 1360 Google Scholar
[26]	Kasturi S, Sivakumar V 2017 Mater. Chem. Front. 1 550 Google Scholar
[27]	Rajendran M, Vaidyanathan S 2020 Chemistry Select 5 5128 Google Scholar
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[29]	Szpikowska-Sroka B, Pawlik N, Goryczka T, Bańczyk M, Pisarski W A 2017 J. Lumin. 188 400 Google Scholar
[30]	Zhang L L, Peng M Y, Dong G P, Qiu J R 2012 Opt. Mater. 34 1202 Google Scholar
[31]	Wen Z X, Li L J, Huang W J, Chen S Y, Lei L, Pang T, Guo H 2022 J. Lumin. 250 119095 Google Scholar
[32]	Kim G C, Park H L, Kim T W 2001 Mater. Res. Bull. 36 1603 Google Scholar
[33]	Hua Y J, Zhang D W, Ma H P, Deng D G, Xu S Q 2016 RSC Adv. 6 113249 Google Scholar
[34]	Meetei S D, Singh S D 2014 J. Lumin. 147 328 Google Scholar
[35]	Liu C J, Zhou Z F, Zhang Y 2019 J. Alloy. Compd. 787 1158 Google Scholar
[36]	Singh N S, Ningthoujam R S, Luwang M N, Singh S D, Vatsa R K 2009 Chem. Phys. Lett. 480 237 Google Scholar
[37]	李瑛, 樊国栋, 阮方毅, 周建锋, 陈茜茜, 王拓 2022 硅酸盐学报 50 2501 Li Y, Fan G D, Ruan F Y, Zhou J F, Chen Q Q, Wang T 2022 J. Chin. Ceram. Soc. 50 2501

Cited By

图 1 (a)—(c) XRD图谱; (d) GTO沿[010]向的晶体结构; (e)稀土(RE)掺入 [GdO₈]十二面体示意图; (f) Dy³⁺, Tb³⁺, Eu³⁺掺杂样品的DSC曲线

Figure 1. XRD patterns of (a) GTO : Dy³⁺, (b) GTO : Tb³⁺ and (c) GTO : Eu³⁺; (d) view of the GTO crystal structure along [010]; (e) [GdO₈] dodecahedron; (f) DSC curves of Dy³⁺, Tb³⁺ and Eu³⁺ doped samples.

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图 2 不同浓度Dy³⁺, Eu³⁺, Tb³⁺掺杂的GTO的SEM图

Figure 2. SEM images of GTO doped with different concentrations of Dy³⁺, Eu³⁺, Tb³⁺.

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图 3 (a) 在575 nm监测下GTO:Dy³⁺的激发光谱图; (b) 在350 nm激发下GTO:Dy³⁺的发射光谱图, 插图为不同Dy³⁺含量荧光粉在575 nm处的荧光强度变化曲线图; (c) 跃迁示意图; (d) GTO:Dy³⁺荧光衰减曲线, 350 nm激发, 在575 nm监测, 插图为寿命随浓度变化曲线

Figure 3. (a) Excitation spectra of GTO:Dy³⁺ monitored at 575 nm; (b) emission spectra of GTO:Dy³⁺ under 350 nm excitation, the inset shows the emission intensity around 575 nm versus concentration; (c) schematic diagram of transitions; (d) decay curves of GTO:Dy³⁺ samples monitored at 575 nm under excitation at 350 nm, inset shows the decay time changing with Dy³⁺ concentration.

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图 4 (a) GTO:Dy³⁺荧光粉在350 nm激发下的色坐标, 插图为样品在365 nm紫外灯照射下的实物发光图; (b) 350 nm激发下, GTO:2.5% Dy³⁺的荧光变温光谱瀑布图; (c) 575 nm的发射峰积分强度与温度的关系折线图

Figure 4. (a) The color coordinates of GTO:Dy³⁺ phosphor at 350 nm excitation. Inset shows the digital images of sample under 365 nm irradiation; (b) temperature dependence PL spectra of GTO:2.5% Dy³⁺ under 350 nm; (c) integrated intensity of 575 nm emission peak at different temperatures.

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图 5 (a) GTO:Eu³⁺在614 nm监测下的激发光谱图; (b) GTO:Eu³⁺在393 nm激发下的发射光谱图, 插图为614 nm处的荧光强度随Eu³⁺掺杂浓度变化线性拟合结果; (c) Eu³⁺能级跃迁示意图; (d) GTO:Eu³⁺在614 nm处监测得到的荧光衰减曲线, 插图表示寿命变化曲线

Figure 5. (a) Excitation spectra of GTO:Eu³⁺ phosphors, monitored at 614 nm; (b) emission spectra of GTO:Eu³⁺ phosphor under 393 nm excitation, the inset shows the linear fitting of emission intensity around 614 nm versus concentration; (c) schematic diagram of transition; (d) decay curves of GTO:Eu³⁺ samples monitored at 614 nm, inset shows the decay time changing with Eu³⁺ concentration.

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图 6 (a) GTO:x% Eu³⁺(x = 0.5—10)在350 nm激发下的色坐标; (b) GTO:7.5% Eu³⁺在393 nm激发下的变温发射光谱图; (c) 614 nm发射峰强度随温度变化曲线

Figure 6. (a) The color coordinates of GTO:x% Eu³⁺( x = 0.5–10) phosphor at 350 nm excitation; (b) temperature dependent PL spectra of GTO:7.5% Eu³⁺ under 393 nm; (c) integrated intensity of 614 nm emission peak at different temperatures.

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图 7 (a) GTO:Tb³⁺荧光粉的激发光谱图; (b) GTO:Tb³⁺荧光粉的发射光谱图; (c) Tb³⁺离子能级跃迁示意图; (d)Tb³⁺荧光衰减曲线, 监测波长为548 nm, 插图表示寿命变化情况

Figure 7. (a) Excitation spectra of GTO:Tb³⁺ phosphors; (b) emission spectra of GTO:Tb³⁺ phosphor; (c) schematic diagram of transitions of Tb³⁺; (d) decay curves of GTO:Tb³⁺ samples, monitored at 548 nm, inset shows the decay time changing with Tb³⁺ concentration.

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图 8 (a) GTO:x%Tb³⁺(x = 0.5—10)荧光粉在377 nm激发下的色坐标; (b) 377 nm激发下, GTO:10%Tb的荧光变温光谱图; (c) 488 nm和545 nm的归一化发射峰强度与温度的关系折线图

Figure 8. (a) The color coordinates of GTO:x% Tb³⁺( x = 0.5–10) phosphor under 377 nm excitation; (b) temperature dependence emission spectra of GTO:7.5% Eu under 393 nm; (c) integrated intensity of 614 nm emission peak at different temperatures.

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图 9 荧光量子产率测试光谱图　(a) GTO:2.5% Dy³⁺; (b) GTO:7.5% Eu³⁺; (c) GTO:10% Tb³⁺; (d) GTO:10% Eu³⁺. 黑色线表示空白样发射光谱, 红色线表示样品发射光谱, 插图为各样品发光波段光谱的放大显示

Figure 9. Fluorescence spectra of phosphors for quantum efficiency measurement: (a) GTO:2.5% Dy³⁺; (b) GTO:7.5% Eu³⁺; (c) GTO:10% Tb³⁺; (d) GTO:10% Eu³⁺. The spectrum of reference is depicted in black and the spectrum of sample is depicted in red. Insets show the amplification of emission spectra.

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表 1 不同材料的发光热稳定性对比

Table 1. Comparison of luminescent thermal stability of different materials.

材料	升温范围/K	热稳定性	文献
GTO:2.5% Dy³⁺	298—473	76%@423 K	This work
BaZn₂(PO₄)₂:Dy³⁺	298—473	77%@423 K	[16]
Ba₂CaWO₆:Dy³⁺	300—500	56%@420 K	[17]
Ca₃Bi(PO₄)₃:Dy³⁺	298—473	54%@473 K	[18]

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表 2 GTO:Eu³⁺的CIE色参数

Table 2. CIE parameters of GTO:Eu³⁺ with different Eu³⁺ doping concentration.

掺杂浓度	CIE色坐标	色温/K	色纯度/%
0.5	(0.53, 0.45)	2197	93.96
1.0	(0.56, 0.43)	1857	96.70
2.5	(0.59, 0.40)	1631	97.17
5.0	(0.60, 0.39)	1621	97.14
7.5	(0.62, 0.37)	1752	97.56
10.0	(0.62, 0.38)	1689	98.51

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表 3 Tb³⁺离子⁵D₄能级荧光衰减寿命拟合值(μs)与平均寿命(μs)

Table 3. Fitting values of lifetimes (μs) and average lifetimes(μs) of Tb³⁺ on ⁵D₄ energy level.

	A₁	τ₁	A₂	τ₂	A₃	τ₃	平均荧光寿命
GTO:0.5%Tb³⁺	18.9	7.5	69.4	46.9	11.0	180.8	95.4
GTO:1.0%Tb³⁺	8.2	3.2	82.3	47.6	9.0	226.4	108.4
GTO:2.5%Tb³⁺	34.6	6.6	52.2	48.3	14.1	199.7	123.2
GTO:5.0%Tb³⁺	41.5	7.1	46.2	51.3	13.5	214.8	134.2
GTO:10%Tb³⁺	21.5	3.9	69.7	48.2	7.3	358.7	181.6

DownLoad: CSV

[1]	McKittrick J, Shea-Rohwer L E 2014 J. Am. Ceram. Soc. 97 1327 Google Scholar
[2]	Fang M H, Bao Z, Huang W T, Liu R S 2022 Chem. Rev. 122 11474 Google Scholar
[3]	孙晓园, 范小暄, 何俊杰, 吕启松, 姜光远, 邓昀, 骆永石, 吴春雷 2020 发光学报 41 265 Google Scholar Sun X Y, Fan X X, He J J, Lv Q S, Jiang G Y, Deng Y, Luo Y S, Wu C L 2020 Chin. J. Lumin. 41 265 Google Scholar
[4]	Zhang X H, Lu Z M, Meng F B, Hu L, Xu X W, Lin J, Tang C C 2012 Mater. Lett. 79 292 Google Scholar
[5]	Yu X F, Yuan D W, Mi X Y 2021 J. Alloys Compd. 857 157585 Google Scholar
[6]	余阳, 刘自军, 陈乔乔, 戴能利, 李进延, 杨旅云 2013 物理学报 62 017804 Google Scholar Yu Y, Liu Z J, Chen Q Q, Dai N L, Li J Y, Yang L Y 2013 Acta Phys. Sin. 62 017804 Google Scholar
[7]	Fang Y C, Huang X R, Juang Y D, Chu S Y 2012 J. Am. Ceram. Soc. 95 1613 Google Scholar
[8]	Christy A G, Mills S J, Kampf A R 2016 Mineral. Mag. 80 415 Google Scholar
[9]	Shannon R D 1976 Acta Crystallogr. 32 751 Google Scholar
[10]	Zhang Z Q, Qin Z T, Zeng L W, Liu J, Li G N, Li C M, Yang J, Capobianco J A, Tang J F 2022 Ceram. Int. 48 13960 Google Scholar
[11]	You P L, Yin G F, Chen X C, Yue B, Huang Z B, Liao X M, Yao Y D 2011 Opt. Mater. 33 1808 Google Scholar
[12]	Jayasimhadri M, Ratnam B V, Jang K, Lee H S, Chen B J, Yi S S, Jeong J H, Moorthy L R 2010 J. Am. Ceram. Soc. 93 494 Google Scholar
[13]	Bedyal A K, Kumar V, Prakash R, Ntwaeaborwa O M, Swart H C 2015 Appl. Surf. Sci. 329 40 Google Scholar
[14]	Ratnam B V, Jayasimhadri M, Jang K, Lee H S, Yi S S, Jeong J H 2010 J. Am. Ceram. Soc. 93 3857 Google Scholar
[15]	Gupta S K, Zuniga J P, Abdou M, Thomas M P, Goonatilleke M D A, Guiton B S, Mao Y B 2020 Chem. Eng. J. 379 122314 Google Scholar
[16]	Li W L, Chen Z Y, Zhang B, Zhao P J, Fan Y W 2022 J. Lumin. 246 118824 Google Scholar
[17]	Yu R J, Shin D S, Jang K W, Guo Y, Noh H M, Moon B K, Choi B C, Jeong J H, Yi S S 2014 Spectrochim. Acta A Mol. Biomol. 125 458 Google Scholar
[18]	Sahu M K, Mula J 2019 J. Am. Ceram. Soc. 102 6087 Google Scholar
[19]	赵旺, 平兆艳, 郑庆华, 周薇薇 2018 物理学报 67 247801 Google Scholar Zhao W, Ping Z Y, Zheng Q H, Zhou W W 2018 Acta Phys. Sin. 67 247801 Google Scholar
[20]	Zhang S Y, Wei D L, Zhu R, Huang Y L, Seo H J 2011 Ceram. Int. 37 3697 Google Scholar
[21]	李兆, 王永锋, 曹静, 吴坤尧, 王亚楠 2020 光谱学与光谱分析 40 3077 Li Z, Wang Y F, Cao J, Wu K Y, Wang Y N 2020 Spectrosc. Spect. Anal. 40 3077
[22]	G. Blasse 1968 Phys. Lett. A 28 444 Google Scholar
[23]	Mahakingam V, Mangiarini F, Vetrone F, Venkatramu V, Bettinelli M, Speghini A, Capobianco J A 2008 J. Phys. Chem. C 112 17745 Google Scholar
[24]	McCamy C S 1992 Color Res. Appl. 17 142 Google Scholar
[25]	Wu Y F, Nien Y T, Wang Y J, Chen I G 2012 J. Am. Ceram. Soc. 95 1360 Google Scholar
[26]	Kasturi S, Sivakumar V 2017 Mater. Chem. Front. 1 550 Google Scholar
[27]	Rajendran M, Vaidyanathan S 2020 Chemistry Select 5 5128 Google Scholar
[28]	续卓, 郭竞渊, 熊正烨, 唐强, 高沐 2021 物理学报 70 167801 Google Scholar Xu Z, Guo J Y, Xiong Z Y, Tang Q, Gao M 2021 Acta Phys. Sin. 70 167801 Google Scholar
[29]	Szpikowska-Sroka B, Pawlik N, Goryczka T, Bańczyk M, Pisarski W A 2017 J. Lumin. 188 400 Google Scholar
[30]	Zhang L L, Peng M Y, Dong G P, Qiu J R 2012 Opt. Mater. 34 1202 Google Scholar
[31]	Wen Z X, Li L J, Huang W J, Chen S Y, Lei L, Pang T, Guo H 2022 J. Lumin. 250 119095 Google Scholar
[32]	Kim G C, Park H L, Kim T W 2001 Mater. Res. Bull. 36 1603 Google Scholar
[33]	Hua Y J, Zhang D W, Ma H P, Deng D G, Xu S Q 2016 RSC Adv. 6 113249 Google Scholar
[34]	Meetei S D, Singh S D 2014 J. Lumin. 147 328 Google Scholar
[35]	Liu C J, Zhou Z F, Zhang Y 2019 J. Alloy. Compd. 787 1158 Google Scholar
[36]	Singh N S, Ningthoujam R S, Luwang M N, Singh S D, Vatsa R K 2009 Chem. Phys. Lett. 480 237 Google Scholar
[37]	李瑛, 樊国栋, 阮方毅, 周建锋, 陈茜茜, 王拓 2022 硅酸盐学报 50 2501 Li Y, Fan G D, Ruan F Y, Zhou J F, Chen Q Q, Wang T 2022 J. Chin. Ceram. Soc. 50 2501

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Vol. 72, Issue 1 - 2023-01-05

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Synthesis and luminescent properties of rare earths doped Gd₂Te₄O₁₁ tellurite phosphors

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Corresponding author: Tang Jian-Feng, tangjf@swu.edu.cn

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