Effect of Gd doping on the structure, dielectric and multiferroic properties of 0.7BiFe0.95Ga0.05O3-0.3BaTiO3 ceramics

Yang Ru-Xia; Lu Yu-Ming; Zeng Li-Zhu; Zhang Lu-Jia; Li Guan-Nan

doi:10.7498/aps.69.20200175

Abstract

The 0.7Bi_1–xGd_xFe_0.95Ga_0.05O₃-0.3BaTiO₃ (BG_xFG-BT, x = 0, 0.05, 0.1, 0.15, 0.2) ceramics were successfully synthesized via the conventional solid-state reaction method. The effects of Gd doping on crystal structure, microstructure, dielectric, ferroelectric and magnetic properties were systematically investigated. X-ray diffraction analysis indicates that Gd doping induce a structural transition from rhombohedral (R3c) to pseudo-cubic (P4mm) in BG_xFG-BT ceramics. Scanning electron microscopy results show a decrease of grain size with doping Gd in BFG-BT. The average grain sizes of the ceramics range from 3.2 μm to 6.2 μm. The dielectric constant and loss tangent are drastically increased and reduced respectively with introducing Gd into the ceramics. Temperature dependent dielectric constant presents a broad peak in the vicinity of Néel temperature (T_N) for all the samples, signifying strong magnetoelectric coupling. An increment in T_N is also observed as a result of Gd-doping in the temperature regions of 230 to 340 ℃. The leakage current density is reduced by about two orders of magnitude under the electric field of 20 kV/cm. This can be ascribed to the reduction of the oxygen vacancy concentration, which is confirmed by the X-ray photoelectron spectroscopy result. The ferroelectricity and ferromagnetism are also improved after the addition of Gd seen from the polarization hysteresis (P-E ) loops and the magnetization hysteresis (M-H) loops. The greatly enhanced magnetism with M_r= 0.0186 emu/g and M_s = 1.084 emu/g is obtained in the ceramic with x = 0.2, almost three point six times larger than that of the undoped ceramic.

Keywords:

Authors and contacts

1.
School of Physical Science and Technology, Southwest University, Chongqing 400715, China
2.
Faculty of Materials and Energy, Southwest University, Chongqing 400715, China

Corresponding author: Lu Yu-Ming, ymlu@swu.edu.cn ; Li Guan-Nan, liguannan@swu.edu.cn

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References

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[2]	Hur N, Park S, Sharma P A, A hn, J S, Guha S, Cheong S W 2004 Nature 429 392 Google Scholar
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Cited By

图 1 (a) BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2)陶瓷的XRD图谱; 样品在(b) 32°, (c) 39.5°和(d) 45.7°附近局部放大图

Figure 1. (a) XRD patterns of BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2) ceramics. Enlarged view of peaks at (b) 32°, (c) 39.5° and (d) 45.7°.

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图 2 BG_xFG - BT陶瓷样品的XRD精修图谱　(a) x = 0; (b) x = 0.1. 红色线、蓝色线和绿色线表示实验值、计算值及二者差值, 短竖线表示布拉格位置

Figure 2. XRD refinement of the BG_xFG - BT ceramics: (a) x = 0, (b) x = 0.1. The red, blue, and green indicatethe experimental, calculated and difference value, respectively. The short bars indicate the positions of Bragg positions.

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图 3 BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2)陶瓷的SEM图像　(a) x = 0; (b) x = 0.05; (c) x = 0.1; (d) x = 0.15; (e) x = 0.2; (f)平均晶粒尺寸随掺杂量变化的关系

Figure 3. The SEM images of BG_xFG - BT ceramics: (a) x = 0; (b) x = 0.05; (c) x = 0.1; (d) x = 0.15; (e) x = 0.2; (f) the composition dependence of average grain size.

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图 4 BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2)陶瓷的XPS图谱　(a) Bi 4f; (b) Fe 2p

Figure 4. XPS spectra of the (a) Bi 4f and (b) Fe 2p lines of BG_xFG - BT (x = 0, 0.05, 0.1, 0.15 and 0.2) ceramics.

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图 5 BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2)陶瓷样品在频率10 kHz, 100 kHz和1 MHz下的ε_r和tan δ随温度的变化　(a) x = 0; (b) x = 0.05; (c) x = 0.1; (d) x = 0.15; (e) x = 0.2

Figure 5. Variation of ε_r and tan δ with temperature at frequencies 10 kHz, 100 kHz and 1 MHz for BG_xFG - BT: (a) x = 0, (b) x = 0.05, (c) x = 0.1, (d) x = 0.15, (e) x = 0.2.

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图 6 室温下BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2)陶瓷样品　(a) 漏电流J随电场E的变化和(b) log J随log E的变化

Figure 6. Leakage current density J of the BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2) ceramic samples as a function of the electric field E at room temperature: (a) J vs E; (b) log J vs log E

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图 7 BG_xFG - BT陶瓷在室温下的电滞回线　(a) x = 0; (b) x = 0.05—0.2

Figure 7. Polarization versus electric field hysteresis loops of BG_xFG - BT ceramics at room temperature: (a) x = 0, (b) x = 0.05–0.2.

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图 8 BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2)陶瓷在室温下的磁滞回线

Figure 8. The room temperature M-H loops of the BG_xFG - BT (x = 0, 0.05, 0.1, 0.15, 0.2) ceramics.

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表 1 Rietveld精修获得的BG_xFG-BT (x = 0, 0.05, 0.1, 0.15, 0.2)陶瓷的晶胞参数

Table 1. The lattice parameters obtained by Rietveld refinement for BG_xFG-BT (x = 0, 0.05, 0.1, 0.15, 0.2).

x	a/Å	b/Å	c/Å	V/Å³	ρ/g·cm^–3	R_wp/%	d/%
0	5.6428(5)	5.6428(5)	13.8896(16)	303.01(6)	7.601(8)	11.2	96.41
0.05	3.9886(4)	3.9886(4)	3.9923(11)	63.51(3)	7.508(4)	10.8	99.28
0.1	3.9879(3)	3.9879(3)	3.9902(15)	63.46(3)	7.454(3)	12.3	98.91
0.15	3.9875(4)	3.9875(4)	3.9899(8)	63.44(2)	7.421(4)	13.8	98.68
0.2	3.9872(6)	3.9872(6)	3.9890(11)	63.41(2)	7.377(3)	15.6	98.63

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[1]	Cheong S W, Mostovoy M 2007 Nat. Mater. 6 13 Google Scholar
[2]	Hur N, Park S, Sharma P A, A hn, J S, Guha S, Cheong S W 2004 Nature 429 392 Google Scholar
[3]	Fina I, Dix N, Fàbrega L, Sánchez F, Fontcuberta J 2010 Thin Solid films 518 4634 Google Scholar
[4]	Zhao T, Scholl A, Zavaliche F, Lee K, Barry M, Doran A, Cruz M P, Chu Y H, Ederer C, Spaldin N A, Das R R, Kim D M, Baek S H, Eom C B, Ramesh R 2006 Nat. Mater. 5 823 Google Scholar
[5]	Patankar K K, Patil S A, Sivakumar K V, Mahajan R P, Kolekar Y D, Kothale M B 2000 Mater. Chem. Phys. 65 97 Google Scholar
[6]	宋骁, 高兴森, 刘俊明 2018 物理学报 67 157512 Google Scholar Song X, Gao X S, Liu J M 2018 Acta Phys. Sin. 67 157512 Google Scholar
[7]	Wang J, Neaton J B, Zheng H, Nagarajan V, Ogale S B, Liu B, Viehland D, Vaithyanathan V, Schlom D G 2003 Science 299 1719 Google Scholar
[8]	Cheng J R, Li N, Cross L E 2003 J. Appl. Phys. 94 5153 Google Scholar
[9]	Pradhan S K, Roul B K 2011 J. Phys. Chem. Solids 72 1180 Google Scholar
[10]	Kumar A, Sharma P, Yang W B, Shen J D, Varshney D, Li Q 2016 Ceram. Int. 42 14805 Google Scholar
[11]	Wang T, Song S H, Ma Q, Tan M L, Chen J J 2019 J. Alloys Comp. 795 60 Google Scholar
[12]	Thakur S, Rai R, Tiwari A 2014 Solid State Commun. 197 1 Google Scholar
[13]	Makoed I I, Amirov A A, Liedienov N A, Pashchenko A V, Yanushkevich K I, Yakimchuk D V, Kaniukov E Y 2019 J. Magn. Magn. Mater. 489 165379 Google Scholar
[14]	Wang K, Si N, Zhang Y L, Zhang F, Guo A B, Jiang W 2019 Vacuum 165 105 Google Scholar
[15]	Ivanova T L, Gagulin V V 2002 Ferroelectrics 265 241 Google Scholar
[16]	Kumar M M, Srinath S, Kumar G S, Suryanarayana S V 1998 J. Magn. Magn. Mater. 188 203 Google Scholar
[17]	Sharma S, Siqueiros J M, Srinet G, Kumar S 2018 J. Alloys Comp. 732 666 Google Scholar
[18]	Hang Q M, Xing Z B, Zhu X H, Yu M, Song Y, Zhu J M, Liu Z G 2012 Ceram. Int. 3 8 Google Scholar
[19]	Wei Y X, Wang X T, Jia J J, Wang X L 2012 Ceram. Int. 38 3499 Google Scholar
[20]	Yang H B, Zhou C G, Liu X Y, Zhou Q, Chen G H, Wang H, Li W Z 2012 Mater. Res. Bull. 47 4233 Google Scholar
[21]	Buscaglia M T, Mitoseriu L, Buscaglia V, Pallecchi I, Viviani M, Nanni P, Siri A S 2006 J. Eur. Ceram. Soc. 26 3027 Google Scholar
[22]	Zhou Y N, Guo T T, Chen J, Liu X Q, Chen X M 2020 J. Alloys Comp. 819 153031 Google Scholar
[23]	Zhao H T, Yang R X, Li Y, Liu G, Lu Y M, Tang J F, Zhang S, Li G N 2020 J. Magn. Magn. Mater. 494 165779 Google Scholar
[24]	Liu X H, Xu Z, Qu S B, Wei X Y, Chen J L 2007 Chin. Sci. Bull. 52 2747 Google Scholar
[25]	Pradhan S K, Das J, Rout P P, Das S K, Mishra D K, Sahu D R, Pradhan A K, Srinivasu V V, Nayak B B, Verma s, Roul V K 2010 J. Magn. Magn. Mater. 322 3614 Google Scholar
[26]	Mukherjee A, Basu S, Manna P K, Yusuf S M, Pal M 2014 J. Alloys Comp. 598 142 Google Scholar
[27]	Kumar M M, Srinivas A, Suryanarayana S V 2000 J. Appl. Phys. 87 855 Google Scholar
[28]	Kumar M, Yadav K L 2007 Appl. Phys. Lett. 91 242901 Google Scholar
[29]	Kumar K S, Venkateswaran C, Kannan D, Tiwari B, Rao M S R 2012 J. Phys. D: Appl. Phys. 45 415302 Google Scholar
[30]	Deng X Z, Zhang J, Zhang S T 2017 J. Mater. Sci: Mater. Electron. 28 2435 Google Scholar
[31]	Deng X L, Wang W, Gao R L, Cai W, Chen G, Fu C L 2018 J. Mater. Sci: Mater. Electron. 29 6870 Google Scholar
[32]	Godara S, Sinha N, Kumar B 2016 Ceram. Int. 42 1782 Google Scholar
[33]	Gowrishankar M, Babu D R, Madeswaran S 2016 J. Magn. Magn. Mater. 418 54 Google Scholar
[34]	Cai W, Fu C L, Gao J C, Chen H Q 2009 J. Alloys Comp. 480 870 Google Scholar
[35]	Chakrabarti C, Fu X H, Qiu Y, Yuan S L, Li C L 2020 Ceram. Int. 46 212 Google Scholar
[36]	Qian G Y, Zhu C M, Wang LG, Tian Z M, Yin C Y, Yuan S L 2017 J. Electron. Mater. 46 6717 Google Scholar
[37]	Song G L, Song Y C, Su J, Song X H, Zhang N, Wang T X, Chang F G 2017 J. Alloys Comp. 696 503 Google Scholar
[38]	Vashisth B K, Bangruwa J S, Beniwal A, Gairola S P, Kumar A, Singh N, Verma V 2017 J. Alloys Comp. 698 699 Google Scholar
[39]	Wei J, Liu Y, Bai X F, Li C, Liu Y L, Xu Z, Gemeiner P, Haumont R, Infante I C, Dkhil B 2016 Ceram. Int. 42 13395 Google Scholar
[40]	Scott J F 2008 J. Phys: Condens. Matter 20 021001 Google Scholar
[41]	Upadhyay S K, Reddy V R, Lakshmi N 2013 J. Asian Ceram. Soc. 1 346 Google Scholar
[42]	Damerdji N O, Amrani B, Khodja K D, Aubert P 2018 J. Supercond. Novel Magn. 31 2935 Google Scholar
[43]	Cao L Z, Cheng B L, Wang S Y, Fu W Y, Ding S, Sun Z H, Yuan H T, Zhou Y L, Chen Z H, Yang G Z 2006 J. Phys. D: Appl. Phys. 39 2819 Google Scholar
[44]	Yu J, Chu J 2008 Sci. Bull. 53 2097 Google Scholar
[45]	Hasan M, Basith M A, Zubair M A, Hossain M S, Mahbub R, Hakim M A, Islam M F 2016 J. Alloys Comp. 687 701 Google Scholar
[46]	Xing Q, Han Z, Zhao S 2017 J. Mater. Sci: Mater. Electron. 28 295 Google Scholar

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Effect of Gd doping on the structure, dielectric and multiferroic properties of 0.7BiFe_0.95Ga_0.05O₃-0.3BaTiO₃ceramics

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Corresponding author: Lu Yu-Ming, ymlu@swu.edu.cn ; Li Guan-Nan, liguannan@swu.edu.cn

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