Effects of Nd-doping on multiferroic properties of Bi6−xNdxFe1.4Ni0.6Ti3O18 polycrystalline

Chen Cheng; Lu Jian-An; Du Wei; Wang Wei; Mao Xiang-Yu; Chen Xiao-Bing

doi:10.7498/aps.68.20181287

Abstract

Single phase polycrystalline Nd-modified BNFNT-x series samples are obtained from the precursors of the same chemical formula, and prepared by using the citric acid-nitrate method. The X-ray photoelectron spectroscopy measurement indicates that a slight Nd modification does not exert significant influence on the stability of the octahedral FeO₆, nor NiO₆ nor TiO₆. When the molar concentration of Nd exceeds 0.25, the stability of BiO layer is cemented and conducive to the insulating role of BiO layer. It is seen that a small quantity of Nd substitution for bismuth can improve the ferroelectric polarization (2P_r) of ～ 19.7 $ \mu {\rm C/cm }^2$. The room-temperature magnetization (2M_s) can reach a maximal value of ～ 4.132 emu/g (1 emu/g = 10⁻³ A·m²/g)in the BNFNT-0.20 sample. Two anomalies are observed in the temperature-dependent dielectric loss spectrum: one is situated in the temperature range from 200 K to 400 K and the other is located in the vicinity of 900 K. It is considered that the loss anomaly found near 900 K might be associated with the viscous motion of ferroelectric domain walls. In addition, the loss peak shown in a temperature range from 200 K to 400 K shifts toward the higher temperature with measuring frequency increasing, indicating the characteristics of dielectric relaxor behavior. The activation energy is evaluated to be 0.287−0.366 eV, which suggests that the relaxor is associated with the electrons transfer and hop between Fe³⁺ and Fe²⁺. The room-temperature magnetization (2M_s) has reached a maximal value of ～ 4.132 emu/g in the BNFNT-0.20 sample. The lattice distortion due to the introduction of Nd changes the angle of such antiferromagnetic coupling bonds as Fe³⁺—O—Fe³⁺, Fe³⁺—O—Ni³⁺ and Ni³⁺—O—Ni³⁺, which leads the AFM spin states to break, and thus increases the magnetic properties. While with further modification of Nd, the drastic lattice distortion reduces the occupation of the B-sites of the magnetic ions, which might be responsible for further deteriorating the magnetic properties.

Keywords:

Authors and contacts

1.
College of Physics Science and Technology, Yangzhou University, Yangzhou 225002, China
2.
Guangling College, Yangzhou University, Yangzhou 225127, China

Corresponding author: Mao Xiang-Yu, xymao@yzu.edu.cn ; Chen Xiao-Bing, xbchen@yzu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51402256, 11374227).

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References

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Cited By

图 2 BNFNT-x (x = 0.00, 0.10, 0.20, 0.25和0.30)样品断面的SEM图像

Figure 2. SEM micrographs of fresh fracture surfaces of BNFNT-x (x = 0.00, 0.10, 0.20, 0.25 and 0.30) samples.

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图 1 室温下BNFNT-x (x = 0.00, 0.10, 0.20, 0.25和0.30)的XRD图谱

Figure 1. XRD patterns of BNFNT-x (x = 0.00, 0.10, 0.20, 0.25 and 0.30) at room temperature.

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图 3 (a) 室温下BNFNT-x样品的拉曼谱; (b) Nd含量对BNFNT-x样品中与BiO层相关的拉曼峰的影响

Figure 3. (a) Raman spectra of BNFNT-x at room temperature; (b) effect of Nd content on Raman peaks associated with BiO layers in BNFNT-x samples.

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图 5 (a) BNFNT-x 样品2P_r-E曲线; (b)电场约为140 kV/cm下Nd含量对2P_r的影响; (c)电场约为190 kV/cm下Nd含量对2P_r的影响

Figure 5. (a) The 2P_r-E curves of BNFNT-x samples; (b) dependence of 2P_rof BNFNT-x ceramics on Nd content x under the electric filed about 140 kV/cm; (c) dependence of 2P_r of BNFNT-x ceramics on Nd content x under the electric filed about 190 kV/cm.

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图 4 室温下BNFNT-x陶瓷样品的电滞回线

Figure 4. Ferroelectric hysteresis loop of BNFNT-x ceramic samples at room temperature.

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图 7 (a)—(e)测量频率为1—492.2 kHz时BNFNT-x样品的介电损耗峰 (插图为BNFNT-x样品相应的激活能)(a) Bi₆Fe_1.4Ni_0.6Ti₃O₁₈; (b) Bi_5.9Nd_0.1Fe_1.4Ni_0.6Ti₃O₁₈; (c) Bi_5.8Nd_0.2Fe_1.4Ni_0.6Ti₃O₁₈; (d) Bi_5.75Nd_0.25Fe_1.4Ni_0.6Ti₃O₁₈; (e) Bi_5.7Nd_0.3Fe_1.4Ni_0.6Ti₃O₁₈; (f) BNFNT-x样品Nd含量对激活能的影响

Figure 7. (a)−(e) Dielectric loss peak with the measurement frequencies from 1 kHz to 492.2 kHz (inset is the corresponding activation energy of BNFNT-x sample): (a) Bi₆Fe_1.4Ni_0.6Ti₃O₁₈; (b) Bi_5.9Nd_0.1Fe_1.4Ni_0.6Ti₃O₁₈; (c) Bi_5.8Nd_0.2Fe_1.4Ni_0.6Ti₃O₁₈;(d) Bi_5.75Nd_0.25Fe_1.4Ni_0.6Ti₃O₁₈; (e) Bi_5.7Nd_0.3Fe_1.4Ni_0.6Ti₃O₁₈; (f) dependence of activation energy of BNFNT-x ceramics on Nd content x.

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图 6 27.17 kHz频率下120—1000 K温度范围内所测量的介电损耗峰(插图为BNFNT-x样品200—400 K的放大部分)

Figure 6. Dielectric loss peak with the measurement temperature from 120 to 1000 K at the frequency of 27.17 kHz. Inset is the corresponding enlarge part of BNFNT-x sample under the temperature from 200 to 400 K.

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图 8 (a)室温下BNFNT-x样品的磁滞回线 (插图为中部放大图像); (b) BNFNT-x样品2M_s随Nd含量的变化

Figure 8. (a) At room temperature, magnetic hysteresis of BNFNT-x samples (inset is the enlarged central part of the M-H curve); (b) dependence of 2M_sof BNFNT-x on the Nd content.

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图 9 BNFNT-x样品的FC和ZFC磁化曲线　(a) x = 0.00; (b) x = 0.10; (c) x = 0.20; (d) x = 0.25; (e) x = 0.30

Figure 9. FC and ZFC magnetization curves of the BNFNT-x sample: (a) x = 0.00; (b) x = 0.10; (c) x = 0.20; (d) x = 0.25; (e) x = 0.30.

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图 10 (a) BNFNT-x样品中Bi的电子能谱图; (b) BNFNT-x样品中Fe的电子能谱图

Figure 10. (a) Electron spectra of Bi in BNFNT-x samples; (b) electron spectra of Fe in BNFNT-x samples.

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map

[1]	Wang J, Neaton J B, Zheng H, Nagarajan V, Ogale S B, Liu B, Vieland D, Vaithyanathan V, Schlom D G, Waghmare U V, Spaldin N A, Rabe K M, Wuttig M, Ramesh R 2003 Science 299 1719 Google Scholar
[2]	Kimura T, Kawamoto S, Yamada Y, Azuma M, Takano M, Tokura Y Y 2003 Phys. Rev. B 67 180401 Google Scholar
[3]	Azuma M, Takata K, Saito T, Ishiwata S, Shimakawa Y, Takano M 2005 J. Am. Chem. Soc. 127 8889 Google Scholar
[4]	Singh R S, Bhimasankaram T, Kumar G S, Suryanarayana S V 1994 Solid State Commun. 91 567 Google Scholar
[5]	Kojima T, Sakai T, Watanabe T, Funakubo H, Saito K, Osada M 2002 Appl. Phys. Lett. 80 2746 Google Scholar
[6]	Noguchi Y, Miyayama M 2001 Appl. Phys. Lett. 78 1903 Google Scholar
[7]	Noguchi Y J, Goshima Y, Miyayama M, Miwa I 2000 Jpn. J. Appl. Phys. 39 L1259 Google Scholar
[8]	Watanabe T, Funakubo H, Osada M, Noguchi Y, Miyayama M 2002 Appl. Phys. Lett. 80 100 Google Scholar
[9]	Yao Y Y, Song C H, Bao P, Su D, Lu X M, Zhu J S, Wang Y N 2004 J. Appl. Phys. 95 3126 Google Scholar
[10]	Kuble F, Schmid H 1992 Ferroelectrics 129 101 Google Scholar
[11]	Mao X Y, Wang W, Chen X B, Lu Y L 2009 Appl. Phys. Lett. 95 082901 Google Scholar
[12]	Liu Z, Yang J, Tang X W, Yin L H, Zhu X B, Dai J M, Sun Y P 2012 Appl. Phys. Lett. 101 122402 Google Scholar
[13]	毛翔宇, 邹保文, 孙慧, 陈春燕, 陈小兵 2015 64 217701 Google Scholar Mao X Y, Zou B W, Sun H, Chen C Y, Chen X B 2015 Acta Phys. Sin. 64 217701 Google Scholar
[14]	Li X N, Zhu Z, Li F, Peng R R, Zhai X F, Fu Z P, Lu Y L 2015 J. Eur. Ceram. Soc. 35 3437 Google Scholar
[15]	Xiong P, Yang J, Qin Y F, Huang W J, Tang X W, Yin L H, Song W H, Dai J M, Zhu X B, Sun Y P 2017 Ceram. Int. 43 4405 Google Scholar
[16]	Fouskove A, Cross L E 1970 J. Appl. Phys. 41 2834 Google Scholar
[17]	Lu W P, Mao X Y, Chen X B 2004 J. Appl. Phys. 95 1973 Google Scholar
[18]	Wang J L, Li L, Peng R R, Fu Z P, Liu M, Lu Y L 2015 J. Am. Ceram. Soc. 98 1528 Google Scholar
[19]	Bai W, Chen C, Yang J, Zhang Y Y, Qi R J, Huang R, Tang X D, Duan C G, Chu J H 2015 Sci. Rep. 5 17846 Google Scholar
[20]	Yu Z H, Yu B Y, Liu Y, Zhou P, Jing J, Lu Y X, Sun H, Chen X B, Ma Z J, Zhang T J, Huang C W, Qi Y J 2017 Ceram. Int. 43 14996 Google Scholar
[21]	Liu S, Yan S Q, Luo H, Yao L L, Hu Z W, Huang S X, Deng L W 2018 J. Mater. Sci. 53 1014 Google Scholar
[22]	Yang J, Yin L H, Liu Z, Zhu X B, Song W H, Dai J M, Yang Z R, Sun Y P 2012 Appl. Phys. Lett. 101 012402 Google Scholar
[23]	Srinivas A, Kumar M M, Suryanarayana S V, Bhimasankaram T 1999 Mater. Res. Bull. 34 989 Google Scholar
[24]	Kim S K, Miyayama M, Yanagida H 1996 Mater. Res. Bull. 31 121 Google Scholar
[25]	Li X N, Ju Z, Li F, Huang Y, Xie Y M, Fu Z P, Knize R J, Lu Y L 2014 J. Mater. Chem. 2 13366 Google Scholar
[26]	Mao X Y, Mao F W, Chen X B 2006 Integr. Ferroelectr. 79 155 Google Scholar
[27]	Yuan B, Yang J, Chen J, Zuo X Z, Yin L H, Tang X W, Zhu X B, Dai J M, Song W H, Sun Y P 2014 Appl. Phys. Lett. 104 062413 Google Scholar
[28]	Wang C H, Liu Z F, Yu L, Tian Z M, Yuan S L 2011 Mater. Sci. Eng. B 176 1243 Google Scholar
[29]	Zuo X Z, Yang J, Song D P, Yuan B, Tang X W, Zhang K J, Zhu X B, Song W H, Dai J M, Sun Y P 2014 J. Appl. Phys. 116 759 Google Scholar
[30]	Shannon R D 1976 Acta Crystallogr. Sect. A 32 751 Google Scholar
[31]	Hussain S, Hasanain S K, Jaffari G H, Faridi S, Rehman F, Abbas T A, Shah S I 2013 J. Am. Ceram. Soc. 96 3141 Google Scholar
[32]	Kojima S, Imaizumi R, Hamazaki S, Takashige M 1994 Jpn J. Appl. Phys. Part 1 33 5559 Google Scholar
[33]	Zhang S T, Chen Y F, Liu Z G, Ming N B 2005 J. Appl. Phys. 97 104106 Google Scholar
[34]	Mao X Y, Sun H, Wang W, Lu Y L, Chen X B 2012 Solid State Commun. 152 483 Google Scholar
[35]	Mao X Y, Wang W, Sun H, Lu Y L, Chen X B 2012 Integr. Ferroelectr. 132 16 Google Scholar
[36]	Wu Y Y, Zhang D M, Yu J, Wang Y B 2009 Mater. Chem. Phys. 113 422 Google Scholar
[37]	Shulman H S, Damjanovic D, Setter N 2000 J. Am. Ceram. Soc. 83 528 Google Scholar
[38]	Bai W, Chen G, Zhu J Y, Yang J, Lin T, Meng X J, Tang X D, Duan C G, Chu J H 2012 Appl. Phys. Lett. 100 082902 Google Scholar
[39]	Ikeda N, Ohsumi H, Ohwada K, Ishii K, Inami T, Kakurai K, Murakami Y, Yoshii K, Mori S, Horibe Y, Kito H 2005 Nature 436 1136 Google Scholar
[40]	Liu Y Y, Chen X M, Liu X Q, Li L 2007 Appl. Phys. Lett. 90 192905 Google Scholar
[41]	Maglione M, Subramanian M A 2008 Appl. Phys. Lett. 93 032902 Google Scholar
[42]	Patwe S J, Achary S N, Manjanna J, Tyagi A K, Deshpande S K, Mishra S K, Krishna P S R, Shinde A B 2013 Appl. Phys. Lett. 103 122901 Google Scholar
[43]	Khomchenko V A, Shvartsman V V, Borisov P, Kleemann W, Kiselev D A, Bdikin I K, Vieira J M, Kholkin A L 2009 Acta Materialia 57 5137 Google Scholar
[44]	Suryanarayana S V, Srinivas A, Singh R S 1999 Proc. SPIE 3903 232 Google Scholar
[45]	雷志威 2015 博士学位论文(合肥: 中国科学技术大学) Lei Z W 2015 Ph. D. Dissertation (Hefei: University of Science and Technology of China) (in Chinese)

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Effects of Nd-doping on multiferroic properties of Bi_6−xNd_xFe_1.4Ni_0.6Ti₃O₁₈ polycrystalline