Preparation, Structural and Electrophysical Studies of Ferroelectric Ceramic Samples of the System (1-2x)BiScO3-xPbTiO3-xPbMg1/3Nb2/3O3, 0 ≤ x ≤ 0.50

Ceramic samples of the (1-2x)BiScO₃-xPbTiO₃-xPbMg_1/3Nb_2/3O₃ system in the whole compositions region x = 0-0.50 were synthesized. According to the X-ray diffraction studies (XRD), the region of solid solutions with perovskite structure formation in the system was determined (x = 0.23-0.50). The presence of a morphotropic phase boundary between tetragonal and rhombohedral forms of solid solutions was established at x = 0.40-0.42. Refined XRD with profile peak analysis established the presence of the additional cubic phase with broadened X-ray reflexes in the solid solutions along with the main phase. It was concluded that the main and additional phases are located in the volume and in the surface layer of ceramic crystallites, respectively. The crystal structures of phases in the polarized and depolarized sample with x = 0.42 were determined by the Rietveld method. It was found that the monoclinic perovskite phase is present in the polarized sample. Temperature-frequency dependences of dielectric permittivity and losses of solid solutions were studied. It was found that the increasing content of BiScO₃ in samples causes a change in their dielectric properties from the usual ferroelectric (FE) in the region (1-2x) = 0-0.08 to ferroelectric-relaxor (FE-R) in the region (1-2x) = 0.08-0.40, and then to the properties of dipole glass with weak correlations in the region (1-2x) > 0.40. It was found that the samples with x = 0.434 and 0.446 below T_c = 414 and 445 K spontaneously pass to the FE state. In the samples with x = 0.42 the application of an electric field of 2.0 kV/ cm induces a transition from FE-R to FE state with T_c = 350 K, which remains after the field is removed.

1. Morphotropic phase boundary perovskites, high strain piezoelectrics, and dielectric ceramics. Ed. by Guo R., Nair K.M., Wong-Ng W., Bhalla A., Viehland D., Suvorov D., Wu C., Hirano S.-I. The American Ceramic Society. Westerville, OH, 2003. 584 p.

2. Handbook of advanced dielectric, piezoelectric and ferroelectric materials: Synthesis, properties and applications. Ed. by Ye Z.-G. Woodhead Publ. Ltd., 2008. 1060 p.

3. Advanced piezoelectric materials. Science and technology. Ed. by K. Uchino. Woodhead Publ. Ltd., 2010. 678 p.

4. Noheda B., Cox D.E., Shirane G., Gao J., Ye Z.-G. Phase diagram of the ferroelectric relaxor (1-x)PbMg1/3Nb2/3O3 - xPbTiO3. Phys. Rev. B. 2002; 66:054104 (10 pages). https://doi.org/10.1103/PhysRevB.66.054104

5. Noheda B., Cox D.E., Shirane G., Guo R., Jones B., Cross L.E. Stability of the monoclinic phase in the ferroelectric perovskite PbZr1-xTixO3. Phys. Rev. B. 2001; 63:014103/1-6. https://doi.org/10.1103/PhysRevB.63.014103

6. Noheda B. Structure and high-piezoelectricity in lead oxide solid solutions. Current Opinion in Solid State and Materials Science. 2002; 6:27-34. https://doi.org/10.1016/S1359-0286(02)00015-3

7. Park S.-E., Shrout T.R. Ultrahigh strain and piezoelectric behavior in relaxor based ferroelectric single crystals. J. Appl. Phys. 1997; 82(4):1804-1811. https://doi.org/10.1063/1.365983

8. Zhang S., Li F. High performance ferroelectric relaxor-PbTiO3 single crystals: Status and perspective. J. Appl. Phys. 2012; 111(3):031301-1-031301-50. https://doi.org/10.1063/1.3679521

9. Sun E., Cao W. Relaxor-based ferroelectric single crystals: Growth, domain engineering, characterization and applications. Prog. Mater. Sci. 2014; 65:124-210. https://doi.org/10.1016/j.pmatsci.2014.03.006

10. Eitel R.E., Randall C.A., Shrout T.R., W. Rehrig P.W., Hackenberger W., Park S.-E. New high temperature morphotropic phase boundary piezoelectrics based on Bi(Me)O3-PbTiO3 ceramics. Jpn. J. Appl. Phys. 2001; 40. Part 1(10):5999-6002.

11. Inaguma Y, Miyaguchi A., Yoshida M., Katsumata T., Shimojo Y, Wang R., Sekiya T. High-pressure synthesis and ferroelectric properties in perovskite-type BiScO3-PbTiO3 solid solution. J. Appl. Phys. 2004; 95(1):231-235. https://doi.org/10.1063/1.1629394

12. Chaigneau J., Kiat J.M., Malibert C., Bogicevic C. Morphotropic phase boundaries in (BiScO3)1-x(PbTiO3)x (0.60<x<0.75) and their relation to chemical composition and polar order. Phys. Rev. B. 2007; 76(9):094111 (7 pages). https://doi.org/10.1103/PhysRevB.76.094111

13. Chen J., Cheng J., Dong S. Review on high temperature piezoelectric ceramics and actuators based on BiScO3-PbTiO3 solid solutions. J. Advanced Dielectrics. 2014; 4(1):1430002 (14 pages). https://doi.org/10.1142/S2010135X14300023

14. Stringer C.J., Donnelly N.J., Shrout T.R., Randall C.A., Alberta E.F., Hackenberger W.S. Dielectric characteristics of perovskite-structured high-temperature relaxor ferroelectrics: The BiScO3-Pb(Mg1/3Nb2/3)O3-PbTiO3 ternary system. J. Am. Ceram. Soc. 2008; 91(6):1781-1787. https://doi.org/10.1103/PhysRevB.84.064113

15. Xie G. Structure and electrical properties of PMN -BS - PT piezoelectric ceramics. Proceed. 2017 Symposium on Piezoelectricity, Acoustic Waves, and Device Applications. October 27-30, 2017. Chengdu, Sichuan, China. P. 537-540.

16. Bush A.A., Kamentsev K.E., Bekhtin M.A., Segalla A.G. Relaxor ferroelectric properties of the (1-2x)BiScO3 xPbTiO3 xPbMg1/3Nb2/3O3 (0.30 ≤ x ≤ 0.46) system. Physics of the Solid State. 2017; 59(1):34-42. https://doi.org/10.1134/S1063783417010036

17. Talanov M.V., Bush A.A., Kamentsev K.E., Sirotinkin V.P., Segalla A.G. Structure-property relationships in BiScO3-PbTiO3-PbMg1/3Nb2/3O3 ceramics near the morphotropic phase boundary. J. Am. Ceram. Soc. 2018; 101(2):683-693. https://doi.org/10.1111/jace.15225

18. Belik A.A., Iikubo S., Kodama K., Igawa N., Shamoto 5., Maie M., Nagai T., Matsui Y., Stefanovich S.Yu., Lazoryak B.I., Takayama-Muromachi E. BiScO3: Centrosymmetric BiMnO3-type oxide. J. Am. Chem. Soc. 2006; 128(3):706-707. https://doi.org/10.1021/ja057574u

19. Krumm S. An interactive Windows program for profile fitting and size/strain analysis. Materials Science Forum. 1996; 228-231:183-190. https://doi.org/10.4028/www.scientific.net/MSF.228-231.183

20. Laugier J., Bochu B. (2003). CELREF. http://www.ccp14.ac.uk/tutorial/lmgp/celref.htm.

21. Le Bail A., Duroy H., Fourquet J.L. Ab-initio structure determination of LiSbWO6 by X-ray powder diffraction. Mat. Res. Bull. 1988; 23:447-452. https://doi.org/10.1016/0025-5408(88)90019-0

22. Rodriguez-Carvajal J. FULLPROF: a program for Rietveld refinement and pattern matching analysis. In: Proceed. of the Satellite Meeting on powder diffraction of the XV Congress of the IUC, Toulouse, France, 1990. P. 127. Available at https://www.ill.eu/sites/fullprof/.

23. Takeuchi T., Ado K., Asai T., Kageyama H., Saito Y, Masquelier Ch., Nakamura O. Thickness of cubic surface phase on barium titanate single-crystalline grains. J. Amer. Ceram. Soc. 1994; 77(6):1665-1668. https://doi.org/10.1111/j.1151-2916.1994.tb09774.x

24. Tunkasiri T., Pakokthom C., Rujijanagul G., Udomporn A. X-ray study of the crystallographic structure of BaTiO3 powder prepared by solid state reaction. Ferroelectrics Lett. Sec. 2000; 28(1-2):29-34.

25. Aoyagi Sh., Kuroiwa Y, Sawada A., Yamashita 1., Atakei T. Composite structure of BaTiO3 nanoparticle investigated by SR X-ray diffraction. J. Phys. Soc. Japan. 2002; 71(5):1218-1221. https://doi.org/10.1143/JPSJ.71.1218

26. Bonneau P, Garnier P., Husson E., Morell A. Structural study of PMN ceramics by X-ray diffraction between 297 and 1023 K. Mat. Res. Bull. 1989; 24(2):201-206. https://doi.org/10.1016/0025-5408(89)90126-8

27. Bonneau P, Garnier P, Calvarin G., Husson E., Gavarri J.R., Morell A. X-ray and neutron diffraction studies of the diffuse phase transition in PbMg1/3Nb2/3O3 ceramics. J. Solid State Chem. 1991; 91(2):350-361. https://doi.org/10.1016/0022-4596(91)90090-5

28. Vakhrushev S., Zhukov S., Fetisov G., Chernyshov V. The high-temperature structure of lead magnoniobate. J. Phys.: Condens. Matter. 1994; 6(22):4021-4027. https://doi.org/10.1088/0953-8984/6/22/001

29. Vakhrushev S.B., Zhukov S.G., Chernyshev V.V. Unique features ofthe crystal structure ofthe (PbMg1/3Nb2/3O3)0 6-(PbTiO3)04 solid solution. Physics of the Solid State. 1999; 41(7):1172-1174. https://doi.org/10.1134/1.1130960

30. Kang B.S., Choi S.K., Park C.H. Diffuse dielectric anomaly in perovskite-type ferroelectric oxides in the temperature range of 400-700 °C. J. Appl. Phys. 2003; 84(3):1904-1911. https://doi.org/10.1063/U589595

31. Bokov A.A., Ye Z.-G. Recent progress in relaxor ferroelectrics with perovskite structure. J. Mat. Sci. 2006; 41(1):31-52. https://doi.org/10.1007/s10853-005-5915-7

32. Phelan D., Stock C., Rodriguez-Rivera J.A., Chi S., Leao J., Long X., Xie Y., Bokov A.A., Ye Z.-G., Ganesh P., Gehring P.M. Role of random electric fields in relaxors. Proc. Natl Acad. Sci. USA. 2014; 111(5):1754-1759. https://doi.org/10.1073/pnas.1314780111

33. Arce-Gamboa J.R., Guzman-Verri G.G. Random electric field instabilities of relaxor ferroelectrics. Quantum Materials. 2017; 2:Article number 28 (7 pages). https://doi.org/10.1038/s41535-017-0032-9