KxNa1–xNbO3:Pr3+铁电体的光致发光和应力发光性能

梁爱华; 王旭升; 李国荣; 郑嘹赢; 江向平; 胡锐

doi:10.7498/aps.71.20220501

摘要

应力发光材料具有应力-光转换特性, 能在机械应力下产生发光, 从而在光学信息显示方面具有很高的应用价值. 本文通过改变铁电基体K_xNa_1–xNbO₃∶0.5%Pr³⁺ (K_xNNOP)的K⁺/Na⁺比来调节材料的晶体结构和缺陷分布, 系统研究了K⁺含量对光致发光和应力发光性能的影响. 研究结果表明, K⁺含量的增加使晶体对称性提高, 导致K_xNNOP样品的光致发光强度降低. 值得注意的是, 在450 nm的光激发下, 在K⁺含量较高的组分中出现了Pr³⁺电子³P₁→³H₅和³P₀→³H₅能级跃迁引起的发射峰, 这归因于Pr³⁺和Nb⁵⁺之间距离的变化导致Pr-O-Nb内价电子电荷转移态(IVCT)的能级位置不同. 在压缩应力下, K_xNNOP (x = 0, 0.01, 0.02, 0.1) 组分展现出明亮的红色应力发光, 且应力发光强度随K⁺含量的增加而增大, 其中K_0.1NNOP组分表现出最高的强度发射. 特别的是, 其应力发光行为具有可重复性和可恢复性的特征. 通过热释光曲线研究了K_xNNOP样品中的陷阱能级, 揭示了K_0.1NNOP中应力发光的增强可能与K⁺含量变化引起的陷阱密度和陷阱深度的差异有关. 基于这些结果, 建立了一个模型来阐述K_xNNOP中可能的应力发光机理.

关键词:

Abstract

Mechanoluminescent (ML) materials have mechanical-light conversion properties and can generate luminescence under mechanical stress, which makes the ML materials have high application value in optical information display. In this work, the crystal structure and defect distribution are adjusted by changing the K⁺/Na⁺ ratio of the ferroelectric matrix K_xNa_1–xNbO₃∶0.5%Pr³⁺ (K_xNNOP), and the effects of K⁺ content on the photoluminescence (PL) and ML properties are systematically investigated. The research results indicate that as the K⁺ content increases, the symmetry of the crystal is enhanced, leading the PL intensity of the K_xNNOP samples to decrease. It is worth noting that the emission peaks caused by the ³P₁→³H₅ and ³P₀→³H₅ transition at the Pr³⁺ electron level appear in the PL spectra of the components with higher K⁺ content under the light excitation of 450 nm, which is attributed to the different energy level positions of the internal valence electron charge transfer states within Pr-O-Nb, caused by the change in the distance between Pr³⁺ and Nb⁵⁺. Under the compressive stress, the K_xNNOP (x = 0, 0.01, 0.02, 0.1) components exhibit the bright red ML, and the ML intensity increases with the K⁺ content increasing. The K_0.1NNOP component exhibits the highest ML intensity emission. In particular, the ML behavior has the characteristics of repeatability and recoverability. The trap energy levels in the K_xNNOP samples are investigated by thermoluminescence curves, revealing that the enhancement of ML in K_0.1NNOP may be related to the differences in trap density and trap depth, caused by changes in K⁺ content. Based on these results, a model is established to elucidate the possible ML mechanism in K_xNNOP.

Keywords:

作者及机构信息

1.
中国科学院上海硅酸盐研究所, 无机功能材料与器件重点实验室, 上海　200050

2.
中国科学院大学, 材料与光电研究中心, 北京　100049

3.
景德镇陶瓷大学材料科学与工程学院, 江西省先进陶瓷材料重点实验室, 景德镇　333403

4.
同济大学材料科学与工程学院, 功能材料研究实验室, 上海　201804

通信作者: 郑嘹赢, zhengly@mail.sic.ac.cn ; 江向平, jiangxp64@163.com ;

基金项目: 国家重点研发计划(批准号: 2021YFA0716502, 2021YFB3800604)和国家自然科学基金(批准号: 51831010)资助的课题.

Authors and contacts

1.
Key Laboratory of Inorganic Functional Materials and Devices, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

2.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

3.
Jiangxi Key Laboratory of Advanced Ceramic Materials, School of Materials Science and Engineering, Jingdezhen Ceramic University, Jingdezhen 333403, China

4.
Functional Materials Research Laboratory, School of Materials Science and Engineering, Tongji University, Shanghai 201804, China

Corresponding author: Zheng Liao-Ying, zhengly@mail.sic.ac.cn ; Jiang Xiang-Ping, jiangxp64@163.com ;

Funds: Project supported by the National Key R&D Program of China (Grant Nos. 2021YFA0716502, 2021YFB3800604) and the National Natural Science Foundation of China (Grant No. 51831010).

文章全文 : translate this paragraph

参考文献

[1]	Wang X, Zhang H, Yu R, Dong L, Peng D, Zhang A, Zhang Y, Liu H, Pan C, Wang Z L 2015 Adv. Mater. 27 2324 Google Scholar
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[9]	Xu C N, Watanabe T, Akiyama M, Zheng XG 1999 Appl. Phys. Lett. 74 1236 Google Scholar
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[27]	Chen T, Liang R, Li Y, Zhou Z, Dong X J 2017 J. Am. Ceram. Soc. 100 1065 Google Scholar
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[30]	Barandiarán Z, Meijerink A, Seijo L J 2015 Phys. Chem. Chem. Phys. 17 19874 Google Scholar
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[38]	Van den eeckhout K, Bos A J, Poelman D, Smet P F 2013 Phys. Rev. B 87 045126 Google Scholar
[39]	Shalgaonkar C, Narlikar A 1972 J. Mater. Sci. 7 1465 Google Scholar
[40]	Sakai R, Katsumata T, Komuro S, Morikawa T 1999 J. Lumin. 85 149 Google Scholar
[41]	Kang F, Yang X, Peng M, Wondraczek L, Ma Z, Zhang Q, Qiu J 2014 J. Phys. Chem. C 118 7515 Google Scholar
[42]	Kang F, Zhang H, Wondraczek L, Yang X, Zhang Y, Lei D Y, Peng M 2016 Chem. Mater. 28 2692
[43]	Gao Y, Huang F, Lin H, Zhou J, Xu J, Wang Y 2016 Adv. Funct. Mater. 26 3139 Google Scholar
[44]	Akiyama M, Xu C N, Matsui H, Nonaka K, Watanabe T 1999 Appl. Phys. Lett. 75 2548 Google Scholar
[45]	Matsui H, Xu C N, Akiyama M, Watanabe T 2000 Jpn. J. Appl. Phys. 39 6582 Google Scholar
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施引文献

图 1 K_xNa_1–xNbO₃∶Pr³⁺粉末与环氧树脂复合的圆柱体示意图

Fig. 1. Schematic diagram of a cylinder composited with K_xNa_1–xNbO₃∶Pr³⁺ powder and epoxy resin.

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图 2 (a) K_xNNOP 样品的 XRD图谱; (b) 2θ在44º—48º范围内的放大图; (c) NNOP, (d) K_0.5NNOP 样品的 Rietveld结构精修图; (e) 晶格常数随x的变化

Fig. 2. (a) XRD patterns of K_xNNOP samples; (b) magnified view of 2θ in the range 44º–48º; rietveld structural refinement plot of (c) NNOP, (d) K_0.5NNOP sample; (e) change of lattice constants with x.

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图 3 K_xNNOP陶瓷样品的拉曼光谱

Fig. 3. Raman spectra of K_xNNOP ceramics sample.

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图 4 (a) K_xNNOP样品的PLE (λ_em = 612 nm)光谱, 插图是310—410 nm范围内放大归一化的 PLE光谱; (b) K_xNNOP样品的PL (λ_ex = 335 nm)光谱, 插图为¹D₂→³H₄发射峰的相对强度与K⁺含量x的关系; (c) PL (λ_ex = 450 nm) 光谱; (d) K_xNNOP样品中的IVCT能级高度与$ {\mathrm{\chi }}_{\mathrm{o}\mathrm{p}\mathrm{t}}\left({\mathrm{N}\mathrm{b}}^{5+}\right) $/$d({\mathrm{P}\mathrm{r}}^{3+}\text{-}{\mathrm{N}\mathrm{b}}^{5+})$变化关系; (e) 能级位置坐标图, 其中ΔE 是从³P₀能级和 IVCT 能级的交叉处到³P₀ 能级底部之间的距离

Fig. 4. (a) PLE (λ_em = 612 nm) spectra of K_xNNOP samples, the inset is the magnified normalized PLE spectrum in the 310-410 nm range; (b) PL (λ_ex = 335 nm) spectra of K_xNNOP samples, the inset is the relationship between the relative intensity of the ¹D₂→³H₄ emission peak and the K⁺ content x; (c) PL (λ_ex = 450 nm) spectra; (d) relationship between IVCT energy in K_xNNOP samples and $ {\mathrm{\chi }}_{\mathrm{o}\mathrm{p}\mathrm{t}}\left({\mathrm{N}\mathrm{b}}^{5+}\right) $/$d({\mathrm{P}\mathrm{r}}^{3+}\text{-}{\mathrm{N}\mathrm{b}}^{5+})$; (e) configurational coordinate diagram, ΔE is the distance from the intersection of the ³P₀ energy level and the IVCT energy level to the bottom of the ³P₀ energy level.

下载: 全尺寸图片幻灯片

图 5 (a) K_0.1NNOP 样品的ML, AG和PL光谱, 插图为相应样品的发光图像; (b) K_xNNOP (x = 0, 0.01, 0.02, 0.1)复合圆柱体在压缩载荷下的ML响应; (c) K_0.1NNOP复合圆柱体在连续负载下的ML强度衰减曲线; (d) 紫外光照射后ML的可恢复性; (e) K_0.1NNOP样品重复测试4次的ML曲线

Fig. 5. (a) ML, AG and PL spectra of K_0.1NNOP sample, insets are images of various luminescence for corresponding samples; (b) ML responses under compressive load of K_xNNOP (x = 0, 0.01, 0.02, 0.1) composite cylinders; (c) ML intensity decay curve under consecutive load of K_0.1NNOP composite cylinder; (d) recoverability of ML after UV light irradiation; (e) ML curve of K_0.1NNOP sample repeated 4 times.

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图 6 (a) K_xNNOP样品的AG (λ_IR = 365 nm)光谱; (b) K_xNNOP样品的AG衰减曲线; (c) K_xNNOP样品的TL曲线; (d) TL曲线的高斯拟合结果

Fig. 6. (a) AG (λ_IR = 365 nm) spectra of K_xNNOP samples; (b) AG decay curves of K_xNNOP samples; (c) TL curves of K_xNNOP samples; (d) Gaussian fitting results of K_xNNOP samples.

下载: 全尺寸图片幻灯片

图 7 (a) K_0.1NNOP样品的XPS光谱; (b) NNOP和K_0.1NNOP样品O 1s 的XPS光谱

Fig. 7. (a) XPS spectrum of K_0.1NNOP powder sample; (b) XPS spectrum for O 1s of NNOP and K_0.1NNOP powders samples.

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图 8 (a) K_0.1NNOP陶瓷的PFM 振幅蝶形环; (b) K_xNNOP中ML机理的示意图 (CB: 导带, VB: 价带)

Fig. 8. (a) PFM amplitude butterfly loops of K_0.1NNOP ceramic; (b) chematic representation of the ML mechanism in K_xNNOP (CB: conduction band, VB: valence band).

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表 1 K_xNa_1–xNbO₃∶Pr³⁺ (x = 0, 0.01, 0.02, 0.1, 0.3, 0.5)样品Rietveld结构精修参数

Table 1. Rietveld structural refinement parameters of K_xNa_1–xNbO₃∶Pr³⁺ (x = 0, 0.01, 0.02, 0.1, 0.3, 0.5) samples

Samples	x = 0	x = 0.01	x = 0.02	x = 0.1	x = 0.3	x = 0.5
Space group	P2₁ma	Amm2	Amm2	Amm2	Amm2	Amm2
a /Å	5.5690	3.9517	3.9016	3.9187	3.9354	3.9639
b/Å	7.7900	5.6027	5.5446	5.6186	5.6020	5.6570
c /Å	5.5180	5.6589	5.5893	5.5678	5.6316	5.6886
V/Å³	239.39	125.29	120.91	122.59	124.16	127.56
R_p/%	0.08	0.24	0.28	0.21	0.24	0.15
R_wp/%	0.06	0.16	0.20	0.17	0.17	0.11

下载: 导出CSV

表 2 K_xNNOP样品计算得到的IVCT能级高度

Table 2. Calculated IVCT energy heights in K_xNNOP samples.

Composition	χ_opt(Nb⁵⁺)	d (Pr³⁺-Nb⁵⁺)/Å	E_IVCT/cm^–1
x = 0	1.862	3.18	29640
x = 0.02	1.862	3.32	30870
x = 0.1	1.862	3.31	30786
x = 0.3	1.862	3.34	31037
x = 0.5	1.862	3.37	31284

下载: 导出CSV

map

[1]	Wang X, Zhang H, Yu R, Dong L, Peng D, Zhang A, Zhang Y, Liu H, Pan C, Wang Z L 2015 Adv. Mater. 27 2324 Google Scholar
[2]	Jeong S M, Song S, Lee S K, Choi B 2013 Appl. Phys. Lett. 102 051110 Google Scholar
[3]	Terasaki N, Yamada H, Xu C N 2013 Catal. Today. 201 203 Google Scholar
[4]	Jeong S M, Song S, Lee S. K, Ha NY 2013 Adv. Mater. 25 6194 Google Scholar
[5]	Jeong S M, Song S, Joo K I, Kim J, Hwang S H, Jeong J, Kim H 2014 Energy Environ. Sci. 7 3338 Google Scholar
[6]	Peng D, Chen B, Wang F J 2015 ChemPlusChem. 80 1209 Google Scholar
[7]	Chen B, Zhang X, Wang F J 2021 Acc. Mater. Res. 2 364 Google Scholar
[8]	Xu C N, Watanabe T, Akiyama M, Zheng XG 1999 Appl. Phys. Lett. 74 2414 Google Scholar
[9]	Xu C N, Watanabe T, Akiyama M, Zheng XG 1999 Appl. Phys. Lett. 74 1236 Google Scholar
[10]	Wang X, Zhang H, Yu R, Dong L, Peng D, Zhang A, Wang Z L 2015 Advanced Materials 27 2324
[11]	Chandra V, Chandra B, Jha P J 2013 Appl. Phys. Lett. 102 241105 Google Scholar
[12]	Wang X, Yamada H, Xu C N. 2005 Appl. Phys. Lett. 86 022905 Google Scholar
[13]	Zhang J C, Pan C, Zhu Y F, Zhao L Z, He H W, Liu X, Qiu J 2018 Adv. Mater. 30 1804644 Google Scholar
[14]	Wei Y, Wu Z, Jia Y, Wu J, Shen Y, Luo H 2014 Appl. Phys. Lett. 105 042902 Google Scholar
[15]	Egerton L, Dillon D M 1959 J. Am. Ceram. 42 438 Google Scholar
[16]	Shirane G, Newnham R, Pepinsky R 1954 Phys. Rev. 96 581 Google Scholar
[17]	Du H, Li Z, Tang F, Qu S, Pei Z, Zhou W J 2006 Mater. Sci. Eng. , B 131 83 Google Scholar
[18]	Fan X H, Zhang J C, Zhang M, Pan C, Yan X, Han W P, Zhang H D, Long Y Z, Wang X J 2017 Opt. Express 25 14238 Google Scholar
[19]	Zhang J C, Fan X H, Yan X, Xia F, Kong W, Long Y Z, Wang X J 2018 Acta Mater. 152 148
[20]	Feng A, Smet P F 2018 Materials 11 484 Google Scholar
[21]	Wang F, Liu X 2009 Chem. Soc. Rev. 38 976 Google Scholar
[22]	Tennery V J, Hang K W 1968 J. Appl. Phy. 39 4749 Google Scholar
[23]	Wells M, Megaw H D 1961 Proc. Phys. Soc. 78 1258 Google Scholar
[24]	Zhang Q, Luo L, Gong J, Du P, Li W P, Yuan G L 2020 J. Eur. 40 3946
[25]	Wang J, Luo L J 2018 J. Am. Ceram. Soc. 101 400 Google Scholar
[26]	Kakimoto K I, Sumi T, Kagomiya I 2010 Jpn J. Appl. Phys. 49 09MD10 Google Scholar
[27]	Chen T, Liang R, Li Y, Zhou Z, Dong X J 2017 J. Am. Ceram. Soc. 100 1065 Google Scholar
[28]	Pinel E, Boutinaud P, Mahiou R J 2004 J. Alloys Compd. 380 225 Google Scholar
[29]	Dorenbos P 2017 Opt. Mater. 69 8 Google Scholar
[30]	Barandiarán Z, Meijerink A, Seijo L J 2015 Phys. Chem. Chem. Phys. 17 19874 Google Scholar
[31]	Sun H, Zhang Q, Wang X, Bulin C 2015 J. Am. Ceram. Soc. 98 601 Google Scholar
[32]	Zhang Q, Sun H, Zhang Y 2014 Jo. Am. Ceram. Soc. 97 868 Google Scholar
[33]	Newman D J, Ng B 2000 Crystal Field Handbook (Cambridge: Cambridge University Press)
[34]	Diallo P, Boutinaud P, Mahiou R, Cousseins J 1997 Phys. Status Solidi A 160 255 Google Scholar
[35]	Li K, Xue D 2006 J. Phys. Chem. A 110 11332 Google Scholar
[36]	Lecointre A, Bessière A, Bos A, Dorenbos P, Viana B, Jacquart S 2011 J. Phys. Chem. C 115 4217 Google Scholar
[37]	Maldiney T, Lecointre A, Viana B, Bessière A, Bessodes M, Gourier D, Richard C, Scherman D 2011 J. Am. Chem. Soc. 133 11810 Google Scholar
[38]	Van den eeckhout K, Bos A J, Poelman D, Smet P F 2013 Phys. Rev. B 87 045126 Google Scholar
[39]	Shalgaonkar C, Narlikar A 1972 J. Mater. Sci. 7 1465 Google Scholar
[40]	Sakai R, Katsumata T, Komuro S, Morikawa T 1999 J. Lumin. 85 149 Google Scholar
[41]	Kang F, Yang X, Peng M, Wondraczek L, Ma Z, Zhang Q, Qiu J 2014 J. Phys. Chem. C 118 7515 Google Scholar
[42]	Kang F, Zhang H, Wondraczek L, Yang X, Zhang Y, Lei D Y, Peng M 2016 Chem. Mater. 28 2692
[43]	Gao Y, Huang F, Lin H, Zhou J, Xu J, Wang Y 2016 Adv. Funct. Mater. 26 3139 Google Scholar
[44]	Akiyama M, Xu C N, Matsui H, Nonaka K, Watanabe T 1999 Appl. Phys. Lett. 75 2548 Google Scholar
[45]	Matsui H, Xu C N, Akiyama M, Watanabe T 2000 Jpn. J. Appl. Phys. 39 6582 Google Scholar
[46]	Zhang H, Yamada H, Terasaki N, Xu C N 2007 Appl. Phys. Lett. 91 081905 Google Scholar
[47]	Fu X, Zheng S, Shi J, Zhang H J 2017 J. Lumin. 192 117 Google Scholar
[48]	Shigemi A, Wada T 2004 Jpn. J. Appl. Phys. 43 6793 Google Scholar
[49]	Wu X, Lin J, Xu Z, Zhao C, Lin C, Wang H, Zhai J 2021 Laser Photonics Rev. 15 2100211 Google Scholar
[50]	Boutinaud P, Sarakha L, Mahiou R 2008 Phys. Condens. Matter 21 025901 Google Scholar
[51]	Xie T, Guo H, Zhang J, He Y, Lin H, Chen G, Zheng Z 2016 J Lumine. 170 150 Google Scholar
[52]	Zhang J C, Long Y Z, Yan X, Wang X, Wang F 2016 Chem. Mater. 28 4052 Google Scholar
[53]	Chandra B P, Chandra V K, Jha P 2015 Phys. B: Condens. Matter 461 38 Google Scholar

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K_xNa_1–xNbO₃:Pr³⁺铁电体的光致发光和应力发光性能

Properties of Photoluminescence and mechanoluminescence of K_xNa_1–xNbO₃:Pr³⁺ ferroelectric

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通信作者: 郑嘹赢, zhengly@mail.sic.ac.cn ; 江向平, jiangxp64@163.com ;

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Corresponding author: Zheng Liao-Ying, zhengly@mail.sic.ac.cn ; Jiang Xiang-Ping, jiangxp64@163.com ;

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