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Multiferroic materials have drawn increasing interest due to the coexistence of ferromagnetism (FM) and ferroelectricity (FE), which provides significant potentials for applications in spintronics, information storage, and sensors, etc. In this paper, the multiferroic Bi6Fe2-xCoxTi3O18 (BFCT-x,x=0-2.0) ceramics are prepared by the solid-state reaction. The BFCT-x samples belong to Aurivillius structure containing five perovskite layers clapped between two Bi-O layers. The lattice constants a, b, and c of BFCT-x samples increase simultaneously with increasing cobalt content up to 0.6 and then decrease with further addition of cobalt. The magnetic and ferroelectric properties, and their corresponding Curie temperatures are measured. At room temperature (RT), the magnetism of the BFCT-0, BFCT-1.8 and BFCT-2.0 samples can be understood by the presence of the antiferromagnetic (AFM) interaction with the dominant paramagnetism (PM) state, which is consistent with the linear behavior of the M-H plot. The Fe3+-O-Fe3+ and Co3+-O-Co3+ interactions present in the BFCT-x samples lead to AFM. The BFCT-0.21.0 samples show saturated magnetic loops, while the BFCT-1.2 sample is far from saturation even under an applied magnetic field of 10 kOe. The M-H curve of BFCT-1.6 sample shows a weak ferromagnetism. The Co content (x=0.2-1.6) dependences of 2Ms and 2Mr have been recorded. Both the 2Ms and 2Mr experience first-increase-then-decrease variation tendency with their maximal values of ～ 4.49 emu/g and ～ 0.89 emu/g located at x =0.6 and x =1.0, respectively. As the cobalt content varies from x=0.2 to x=1.2, the paramagnetic-ferromagnetic phase transition temperature (TMC) decreases from 752 to 372 K. At RT, the BFCT-x samples are ferroelectric, and the maximum and minimum values of remnant polarization (2Pr) are about 8.0 up C/cm2 (x=0.6) and 1.1 up C/cm2(x=1.2), respectively. The 2Pr of the BFCT-0.6 is about three times larger than that of Bi5Fe2Ti3O18 (x=0) sample. Furthermore, the dependence of 2Pr on Co content first increases with Co doping when x qslant 0.6, and decreases from x=0.8 to x=1.2, and then increases again. The ferroelectric Curie temperature Tc of the BFCT-x samples increases with increasing x up to 0.8 and then decreases with further increasing cobalt content. It is noteworthy that the Tc of BFCT-1.0 is 2 K lower than that of BFCT-0.6, while the 2Pr decreases by 63%. It is seen that the 2Pr and 2Mr increase simultaneously with increasing Co content (below 0.6). When 0.8 x qslant 1.0, the 2Mr increases while 2Pr decreases with increasing Co content. After x1.2, the 2Mr decreases while 2Pr increases with increasing Co content. The repelling between the FE and FM as discussed above may result from the magnetic-crystalline and ferroelectric-crystalline anisotropy. The mechanism of this phenomenon is not quite clear and needs further investigation.
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Keywords:
- Aurivillius structure /
- ceramics /
- multiferroic /
- dielectric properties
[1] Wang J, Neaton J B, Zheng H, Nagarajan V, Ogale S B, Liu B, Viehland D, Vaithyanathan V, Schlom D G, Waghamare U V, Spaldine N A, Rabe K M, Wattig M, Ramesh R 2003 Science 299 1719
[2] Hill N A 2000 J. Phys. Chem. B 104 6694
[3] Ramesh R, Spaldin N A 2007 Nature Mater. 6 21
[4] Wang K F, Liu J M, Ren Z F 2009 Adv. Phys. 58 321
[5] Dong X W, Wang K F, Wan J G, Zhu J S, Liu J M 2008 J. Appl. Phys. 103 094101
[6] Mao X Y, Wang W, Chen X B, Lu Y L 2009 Appl. Phys. Lett. 95 082901
[7] Snedden A, Hervoches C H, Lightfoot P 2003 Phys. Rve. B 67 092102
[8] Yuan B, Yang J, Song D P, Zuo X Z, Tang X W, Zhu X B, Dai J M, Song W H, Sun Y P 2015 J. Appl. Phys. 117 023907
[9] Patwe S J, Achary S N, Manjanna J, Tyagi A K, Deshpande S K, Mishra S K, Krishna P S R, ShindeA B 2013 Appl. Phys. Lett. 103 122901
[10] Kubel F, Schmid H 1992 Ferroelectrics 129 101
[11] Fouskova A, Cross L E 1970 J. Appl. Phys. 41 2834
[12] Neaton J B, Ederer C, Waghmare U V, Spaldin N A, Rabe K M 2005 Phys. Rev. B 71 014113
[13] Singh R S, Bhimasankararn T, Kumar G S, Suryanarayana S V 1994 Solid State Commun. 91 567
[14] Mao X Y, Wang W, Chen X B 2008 Solid State Commun. 147 186
[15] Hu X, Wang W, Mao X Y, Chen X B 2010 Acta Phys. Sin. 59 8160 (in Chinese) [胡星, 王伟, 毛翔宇, 陈小兵 2010 物理学报 59 8160]
[16] Yang J, Tong W, Liu Z, Zhu X B, Dai J M, Song W H, 1 Yang Z R, Sun Y P 2012 Phys. Rve. B 86 104410
[17] 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
[18] Palizdar M, Comyn T P, Ward M B, Brown A P, Harrington J P, Kulkarni S, Keeney L, Roy S, Pemble M, Whatmore R, Quinn C, Kilcoyne S H, Bell A J 2012 J. Appl. Phys. 112 073919
[19] Chen C Y, Hou S, Mao X Y, Chen X B 2013 Mater. Sci. Forum 745 142
[20] 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
[21] Shannon R D 1976 Acta Crystallogr., Sect. A: Cryst. Phys., Diffr., Theor. Gen. Crystallogr 32 751
[22] Rondinelli J M, Spaldin N A 2009 Phys. Rev. B 79 054409
[23] Song G L, Luo Y P, Su J, Zhou X H, Chang F G 2013 Acta Phys. Sin. 62 097502 (in Chinese) [宋桂林, 罗艳萍, 苏健, 周晓辉, 常方高 2013 物理学报 62 097502]
[24] Cai M Q, Liu J C, Yang G W, Cao Y L, Tan X, Yi X, Wang Y G, Wang L L, Hu W Y 2007 J. Chem. Phys. 126 154708
[25] Zhang H, Liu Y J, Pan L H, Zhang Y 2009 Acta. Phys. Sin. 58 7141 (in Chinese) [张晖, 刘拥军, 潘丽华, 张瑜 2009 物理学报 58 7141]
[26] Sun H, Lu X M, Xu T T, Su J, Jin Y M, Ju C C, Huang F Z, Zhu J S 2012 J. Appl. Phys. 111 124116
[27] Mao X Y, Wei W, Hui S, Lu Y L, Chen X B 2012 J. Mater. Sci. 47 2960
[28] 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
[29] Li J B, Huang Y P, Rao G H, Liu G Y, Luo J, Chen J R, Liang J K 2010 Appl. Phys. Lett. 96 222903
[30] Shimakawa Y, Kubo Y, Nakagawa Y, Goto S, Kamiyama T, Asano H, Izumi F 2000 Phys. Rev. B 61 6559
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[1] Wang J, Neaton J B, Zheng H, Nagarajan V, Ogale S B, Liu B, Viehland D, Vaithyanathan V, Schlom D G, Waghamare U V, Spaldine N A, Rabe K M, Wattig M, Ramesh R 2003 Science 299 1719
[2] Hill N A 2000 J. Phys. Chem. B 104 6694
[3] Ramesh R, Spaldin N A 2007 Nature Mater. 6 21
[4] Wang K F, Liu J M, Ren Z F 2009 Adv. Phys. 58 321
[5] Dong X W, Wang K F, Wan J G, Zhu J S, Liu J M 2008 J. Appl. Phys. 103 094101
[6] Mao X Y, Wang W, Chen X B, Lu Y L 2009 Appl. Phys. Lett. 95 082901
[7] Snedden A, Hervoches C H, Lightfoot P 2003 Phys. Rve. B 67 092102
[8] Yuan B, Yang J, Song D P, Zuo X Z, Tang X W, Zhu X B, Dai J M, Song W H, Sun Y P 2015 J. Appl. Phys. 117 023907
[9] Patwe S J, Achary S N, Manjanna J, Tyagi A K, Deshpande S K, Mishra S K, Krishna P S R, ShindeA B 2013 Appl. Phys. Lett. 103 122901
[10] Kubel F, Schmid H 1992 Ferroelectrics 129 101
[11] Fouskova A, Cross L E 1970 J. Appl. Phys. 41 2834
[12] Neaton J B, Ederer C, Waghmare U V, Spaldin N A, Rabe K M 2005 Phys. Rev. B 71 014113
[13] Singh R S, Bhimasankararn T, Kumar G S, Suryanarayana S V 1994 Solid State Commun. 91 567
[14] Mao X Y, Wang W, Chen X B 2008 Solid State Commun. 147 186
[15] Hu X, Wang W, Mao X Y, Chen X B 2010 Acta Phys. Sin. 59 8160 (in Chinese) [胡星, 王伟, 毛翔宇, 陈小兵 2010 物理学报 59 8160]
[16] Yang J, Tong W, Liu Z, Zhu X B, Dai J M, Song W H, 1 Yang Z R, Sun Y P 2012 Phys. Rve. B 86 104410
[17] 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
[18] Palizdar M, Comyn T P, Ward M B, Brown A P, Harrington J P, Kulkarni S, Keeney L, Roy S, Pemble M, Whatmore R, Quinn C, Kilcoyne S H, Bell A J 2012 J. Appl. Phys. 112 073919
[19] Chen C Y, Hou S, Mao X Y, Chen X B 2013 Mater. Sci. Forum 745 142
[20] 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
[21] Shannon R D 1976 Acta Crystallogr., Sect. A: Cryst. Phys., Diffr., Theor. Gen. Crystallogr 32 751
[22] Rondinelli J M, Spaldin N A 2009 Phys. Rev. B 79 054409
[23] Song G L, Luo Y P, Su J, Zhou X H, Chang F G 2013 Acta Phys. Sin. 62 097502 (in Chinese) [宋桂林, 罗艳萍, 苏健, 周晓辉, 常方高 2013 物理学报 62 097502]
[24] Cai M Q, Liu J C, Yang G W, Cao Y L, Tan X, Yi X, Wang Y G, Wang L L, Hu W Y 2007 J. Chem. Phys. 126 154708
[25] Zhang H, Liu Y J, Pan L H, Zhang Y 2009 Acta. Phys. Sin. 58 7141 (in Chinese) [张晖, 刘拥军, 潘丽华, 张瑜 2009 物理学报 58 7141]
[26] Sun H, Lu X M, Xu T T, Su J, Jin Y M, Ju C C, Huang F Z, Zhu J S 2012 J. Appl. Phys. 111 124116
[27] Mao X Y, Wei W, Hui S, Lu Y L, Chen X B 2012 J. Mater. Sci. 47 2960
[28] 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
[29] Li J B, Huang Y P, Rao G H, Liu G Y, Luo J, Chen J R, Liang J K 2010 Appl. Phys. Lett. 96 222903
[30] Shimakawa Y, Kubo Y, Nakagawa Y, Goto S, Kamiyama T, Asano H, Izumi F 2000 Phys. Rev. B 61 6559
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