Synthesis and long afterglow characteristics of Sr2MgSi2O7:Eu2+, Dy3+ by experimental optimization design

Liu Sheng-Yi; Zhang Jin-Su; Sun Jia-Shi; Chen Bao-Jiu; Li Xiang-Ping; Xu Sai; Cheng Li-Hong

doi:10.7498/aps.68.20182015

Abstract

An optimization method is used to obtain the longest effective afterglow time in the rare earth ions doped long lasting phosphors. The effective afterglow time is defined as the time for the intensity to decays to 10% of the initial intensity. In this paper, we choose the Eu²⁺ and Dy³⁺ coped Sr₂MgSi₂O₇ as the experimental objects. In order to obtain the longest effective afterglow time of Sr₂MgSi₂O₇:Eu²⁺, Dy³⁺ phosphor, the experiment is optimized by quadratic general rotation combination design. The Sr₂MgSi₂O₇:Eu²⁺, Dy³⁺ phosphor are synthesized via a solid-state reaction. The effective afterglow time is obtained by the afterglow decay curve. A binary quadratic regression equation model relating the rare earth ions Eu²⁺/Dy³⁺ doping concentrations to the effective afterglow time is established. The genetic algorithm is used to solve the equation. The optimal doping concentration of Eu²⁺ and Dy³⁺ are 0.5 mol% and 1.0 mol%, respectively. The theoretical maximum value of effective afterglow time is calculated to be 321 s. The phosphor with the optimal doping concentration Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺ are synthesized by the same method as that of synthesizing the frontal samples. The X-ray diffraction shows that the optimal sample prepared is of pure phase, and the doping ions have no effect on the lattice structure of the matrix. A characteristic emission at 465 nm due to the 4f⁶5d¹−4f⁷ transition of Eu²⁺is observed under the 370 nm excitation. The afterglow curve of the optimal sample is measured and the effective afterglow time is 333 s which has a good match with the theoretically calculated value of 321 s. The thermoluminescence spectrum of the optimal phosphor is measured, and the trap depth is calculated to be 0.688 eV according to the Chen’s model. Moreover, the long-lasting luminescence process of Eu²⁺ as the luminescence center of Sr₂MgSi₂O₇ matrix is discussed in the energy level diagram.

Keywords:

Authors and contacts

College of Science, Dalian Maritime University, Dalian 116026, China

Corresponding author: Zhang Jin-Su, melodyzjs@dlmu.edu.cn ; Sun Jia-Shi, sunjs@dlmu.edu.cn ;

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 61604029, 11774042), the Natural Science Foundation of Liaoning Province, China (Grant Nos. 2014025010, 20180510051), the Fundamental Research Funds for the Central Universities, China (Grant Nos. DUT18LK48, 3132018239), the High-level Personnel in Dalian Innovation Support Program, China (Grant No. 2017RQ070), and the Dalian Maritime University Teacher Development Topic, China (Grant No. 2017JFZ04).

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References

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Cited By

图 1 Eu²⁺/Dy³⁺的余辉衰减曲线

Figure 1. Afterglow attenuation curve of Eu²⁺/Dy³⁺.

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图 2 Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺和标准数据卡卡片JCPDS#75-1736的XRD图谱

Figure 2. XRD pattern of Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol%Dy³⁺ and standard data card card JCPDS#75-1736.

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图 3 Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺的荧光激发和发射光谱

Figure 3. Fluorescence excitation and emission spectroscopy of Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺.

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图 4 Sr₂MgSi₂O₇:0.5 mol%Eu²⁺, 1.0 mol% Dy³⁺的余辉衰减曲线

Figure 4. Afterglow decay curve of Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺.

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图 5 Sr₂MgSi₂O₇:0.5 mol%Eu²⁺, 1.0 mol% Dy³⁺的热释发光光谱

Figure 5. Thermoluminescence spectroscopy of Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺.

DownLoad: Full-Size Img PowerPoint

图 6 长余辉发光过程的简单模型

Figure 6. Simple model of long afterglow luminescence process.

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表 1 自然因素水平编码表

Table 1. Natural factor level coding table

Z_j(x_j)	x₁(Eu²⁺)/%	x₂(Dy³⁺)/%
Z_2j(r)	5	10
Z_0j + $\varDelta_j$(1)	4.341	8.682
Z_0j(0)	2.75	5.5
Z_0j – $\varDelta_j$(–1)	1.159	2.318
Z_1j(–r)	0.5	1
$\varDelta_j$ = (Z_2j – Z_1j)/2r	1.591	3.182
x_j = (Z_j – Z_0j)/$\varDelta_j$	x₁ = (Z₁ – 2.75)/1.591	x₂ = (Z₂ – 5.5)/3.182

DownLoad: CSV

表 2 二次通用旋转组合设计实验方案及余辉时间

Table 2. Quadratic general rotation combination design experimental scheme and afterglow time.

Number	x₀	x₁	x₂	x₁x₂	x₁²	x₂²	Afterglow time/s
1	1	1	1	1	1	1	132
2	1	1	–1	–1	1	1	80
3	1	–1	1	–1	1	1	212
4	1	–1	–1	1	1	1	184
5	1	r	0	0	r²	0	116
6	1	–r	0	0	r²	0	290
7	1	0	r	0	0	r²	172
8	1	0	–r	0	0	r²	138
9	1	0	0	0	0	0	141
10	1	0	0	0	0	0	104
11	1	0	0	0	0	0	102
12	1	0	0	0	0	0	101
13	1	0	0	0	0	0	105

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表 3 显著性检验分析

Table 3. Significant test analysis.

	Afterglow time/s
	方差或 t 统计量	显著性水平$\alpha$	显著性水平$\alpha$
x₀	14.490	0.001	***
x₁	5.193	0.01	**
x₂	1.546	0.2	*
x₁x₂	0.703	0.6	Insignificant
x₁²	6.116	0.01	***
x₂²	2.408	0.2	*
F_回	18.07	0.001	***
注: *极显著水平($\alpha$ ≤ 0.01); 显著水平($\alpha$ ≤ 0.1); *较显著水平($\alpha$ ≤ 0.25).

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表 5 Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺的陷阱深度参数

Table 5. Trap depth parameter of Sr₂MgSi₂O₇:0.5 mol% Eu²⁺, 1.0 mol% Dy³⁺.

T₁/K	T_m/K	T₂/K	$\tau$/K	$\delta$/K	$\omega$/K	${\mu _{\rm g}}$/K	${E_\tau }$/eV	${E_\delta }$/eV	${E_\omega }$/eV	E/eV
339*	365	393	26	28	54	0.528	0.673	0.701	0.690	0.688

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表 4 文献[27, 28]的模型陷阱深度参数

Table 4. Model trap depth parameter in Refs. [27, 28].

	$\tau$	$\delta$	$\omega$
${c_\alpha }$	1.81	1.71	3.54
${b_\alpha }$	2	0	1

DownLoad: CSV

map

[1]	Chang C K, Mao D L, Shen J F, Feng C L 2003 J. Alloy. Compd. 348 224 Google Scholar
[2]	Johnson E J, Kafalas J, Dyes W A 1982 Appl. Phys. Lett. 40 993 Google Scholar
[3]	梅屹峰, 唐远河, 梅小宁, 刘汉臣, 刘骞, 余洋, 李宁远, 高恒 2016 65 170701 Google Scholar Mei Q F, Tang Y H, Mei X N, Liu H C, Liu Q, Yu Y, Li N Y, Gao H 2016 Acta Phys. Sin. 65 170701 Google Scholar
[4]	彭玲玲, 曹仕秀, 赵聪, 刘碧桃, 韩涛, 李凤, 黎小敏 2018 67 187801 Google Scholar Peng L L, Cao S X, Zhao C, Liu B T, Han T, Li F, Li X M 2018 Acta Phys Sin. 67 187801 Google Scholar
[5]	刘文全, 朝克夫, 武文杰, 包富泉, 周炳卿 2018 65 207801 Google Scholar Liu W Q, Zhao K F, Wu W J, Bao F Q, Zhou B Q 2018 Acta Phys. Sin. 65 207801 Google Scholar
[6]	Lindmayer J 1988 Solid State Technol. 31 135 Google Scholar
[7]	Fan W H, Wang Y C, Xu H, Li D, Wei Z, Yang B Z, Niu L H 1999 J. Appl. Phys. 85 451 Google Scholar
[8]	Zhang Y, Wang B, Liu X, Xiao M 2010 J. Appl. Phys. 107 103502 Google Scholar
[9]	Yamashita S A, Ogawa N 1989 Phys. States Solidi B 118 89
[10]	Ou Y Y, Zhou W J, Liu C M, Lin L T, Brik G M, Dorenbos P 2018 J. Phys. Chem. C 122 2959 Google Scholar
[11]	Yan J, Liu C M, Vlieland J, Zhou J B, Dorenbos P, Huang Y, Tao Y, Liang H B 2017 J. Lumin. 183 97 Google Scholar
[12]	Liu F, Yan W, Chuang Y J, Zhen Z, Xie J, Pan Z 2013 Sci. Rep. 3 1554 Google Scholar
[13]	Xu X, He Q, Yan L 2013 J. Alloy. Compd. 574 22 Google Scholar
[14]	Wang J, Ma Q, Wang Y, Shen H, Yuan Q 2017 Nanoscale 9 6204 Google Scholar
[15]	孙佳石, 李香萍, 李树伟, 吴金磊, 石琳琳, 徐赛, 张金苏, 程丽红, 陈宝玖 2017 66 100201 Google Scholar Sun J S, Li X P, Wu J L, Li S W, Shi L L, Xu S, Zhang J S, Cheng L H, Chen B J 2017 Acta Phys Sin. 66 100201 Google Scholar
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[17]	任露泉 2009 试验优化设计与分析 (北京: 科学出版社) 第172—185页 Ren L Q 2009 Design of Experiment and Optimization (Beijing: Science Press) pp172–185 (in Chinese)
[18]	王志军, 刘海燕, 杨勇, 蒋海峰, 段平光, 李盼来, 杨志平, 郭庆林 2014 63 077802 Google Scholar Wang Z J, Liu H Y, Yang Y, Jiang H F, Duan P G, Li P L, Yang Z P, Guo Q L 2014 Acta Phys. Sin. 63 077802 Google Scholar
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[20]	翟梓会, 孙佳石, 张金苏, 李香萍, 程丽红, 仲海洋, 李晶晶, 陈宝玖 2013 62 203301 Google Scholar Zhai Z H, Sun J S, Zhang J S, Li X P, Cheng L H, Zhong H Y, Li J J, Chen B J 2013 Acta Phys Sin. 62 203301 Google Scholar
[21]	程仕平, 徐慧, 王德志, 王光君, 吴壮志 2007 稀有金属材料与工程 36 1933 Google Scholar Cheng S P, Xu H, Wang D Z, Wang G J, Wu Z Z 2007 Rare Metal. Mat. Eng. 36 1933 Google Scholar
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[23]	Xiong W W, Yin C L, Zhang Y, Zhang J L 2009 Chin. J. Mech. Eng-En. 22 862 Google Scholar
[24]	Tan G Z, Zhou D M, Jiang B J, Dioubate M I 2008 J. Cent. South Univ. Technol. 15 845 Google Scholar
[25]	石琳琳, 孙佳石, 翟梓会, 李香萍, 张金苏, 陈宝玖 2014 光子学报 43 1116002 Shi L L, Sun J S, Zhai Z H, Li X P, Zhang J S, Chen B J 2014 Acta Photo. Sin. 43 1116002
[26]	Wu H, Hu Y, Chen L, Wang X 2011 J. Alloy. Compd. 509 4304 Google Scholar
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[28]	张哲, 徐旭辉, 邱建备, 张新, 余雪 2014 光谱学与光谱分析 34 1486 Google Scholar Zhang Z, Xu X H, Qiu J B, Zhang X, Yu X 2014 Spetroscopy Spectral Anal. 34 1486 Google Scholar
[29]	齐智坚, 黄维刚 2013 62 197801 Google Scholar Qi Z J, Huang W G 2013 Acta Phys Sin. 62 197801 Google Scholar

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Synthesis and long afterglow characteristics of Sr₂MgSi₂O₇:Eu²⁺, Dy³⁺ by experimental optimization design

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Corresponding author: Zhang Jin-Su, melodyzjs@dlmu.edu.cn ; Sun Jia-Shi, sunjs@dlmu.edu.cn ;

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