Comprehensive Analysis of Preparation Techniques, Structural Features, and Properties in Composite Multiferroic Systems
Keywords:
Composite multiferroics; magnetoelectric coupling; synthesis-structure-property relationship; hydrothermal synthesis; phase interface; ferroelectricity; ferromagnetism.Abstract
This empirical study provides a comprehensive exploration of synthesis methodologies, characterization techniques, and fundamental properties in composite multiferroic materials. Multiferroics, exhibiting simultaneous ferroelectric and magnetic ordering, represent a frontier class of multifunctional materials with significant technological potential. Through systematic investigation of 127 distinct composite samples synthesized via solid-state reaction, sol-gel, and hydrothermal methods, we establish critical correlations between processing parameters and resultant multiferroic properties. X-ray diffraction, scanning electron microscopy, and vibrating sample magnetometry analyses reveal distinct phase formation behavior dependent on synthesis route, with optimal magnetoelectric coupling coefficients (up to 18.7 mV/cm·Oe) achieved in samples with controlled interfaces between ferroelectric and ferromagnetic components. Statistical analysis demonstrates significant variations in multiferroic performance across synthesis methods (p<0.001), with hydrothermal processing yielding superior magnetization (1.27±0.11 emu/g) while maintaining comparable ferroelectric properties to conventional techniques. These findings establish comprehensive synthesis-structure-property relationships in composite multiferroics, providing quantitative
guidance for optimizing magnetoelectric coupling in next-generation multifunctional devices.
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References
1. J. van Suchtelen, "Product properties: a new application of composite materials," Philips Res. Rep., vol. 27, no. 1, pp. 28-37, 1972.
2. J. Ryu, A. V. Carazo, K. Uchino, and H. E. Kim, "Magnetoelectric properties in piezoelectric and magnetostrictive laminate composites," Jpn. J. Appl. Phys., vol. 40, no. 8, pp. 4948-4951, 2001.
3. H. Zheng et al., "Multiferroic BaTiO₃-CoFe₂O₄ nanostructures," Science, vol. 303, no. 5658, pp. 661-663, 2004.
4. J. Wan, X. Wang, Y. Li, and J. Liu, "Structural and electrical properties of BaTiO₃-CoFe₂O₄ composites prepared by spark plasma sintering," J. Appl. Phys., vol. 116, no. 4, p. 044106, 2014.
5. S. Ren, M. Wuttig, and M. Bedzyk, "Epitaxial integration of ferromagnetic and ferroelectric materials," Science, vol. 315, no. 5810, pp. 954-957, 2007.
6. Y. Liu, Y. Wu, D. Li, Y. Zhang, J. Zhang, and J. Yang, "A study of structural, ferroelectric, ferromagnetic, dielectric properties of NiFe₂O₄-BaTiO₃ multiferroic composites," J. Mater. Sci.: Mater. Electron., vol. 24, no. 6, pp. 1900-1904, 2013.
7. W. Zhang, N. Gao, J. He, C. Shen, D. Wu, and Y. Xie, "Theoretical predictions for magnetoelectric coupling in composite multiferroics with tailored interfaces," Acta Mater., vol. 125, pp. 65-75, 2017.
8. T. Zhang, X. Li, J. Dai, A. Yang, and Y. Tan, "Strain-mediated magnetoelectric coupling in BiFeO₃-NiFe₂O₄ particulate composites," J. Magn. Magn. Mater., vol. 377, pp. 100-104, 2015.
9. J. Chen, Z. Xu, X. Qu, and Q. Huang, "Preparation and properties of BiFeO₃-CoFe₂O₄-PbTiO₃ multiferroic composite ceramics," J. Alloys Compd., vol. 710, pp. 275-284, 2017.
10. L. Liu, S. Zhang, Y. Wang, Y. Guo, and J. Zhang, "Enhanced magnetoelectric properties of hydrothermally synthesized BiFeO₃-NiFe₂O₄ composites with controlled interfaces," J. Mater. Chem. C, vol. 6, no. 8, pp. 2076-2086, 2018.
11. Q. Wang, X. Wang, X. Liu, and J. Zhu, "Strain-mediated magnetoelectric effect in particulate compositionally graded BaTiO₃-CoFe₂O₄ composites," J. Am. Ceram. Soc., vol. 99, no. 7, pp. 2425-2432, 2016.
12. M. Zhou, Y. Li, S. Cai, L. Shan, and X. Liu, "Enhanced magnetoelectric coupling in sol-gel derived 3-1 type multiferroic composites with tailored microstructure," Ceram. Int., vol. 44, no. 1, pp. 4364-4372, 2018.
13. Y. Liu et al., "Hydrothermal synthesis and enhanced magnetoelectric properties of BiFeO₃-NiFe₂O₄ composites with adjustable interfaces," J. Mater. Chem. C, vol. 7, no. 3, pp. 764-773, 2019.
14. R.C. Kambale, D.Y. Jeong, and J. Ryu, "Current status of magnetoelectric composite thin/thick films," Adv. Cond. Matter Phys., vol. 2012, p. 824643, 2012.
15. C. Israel, N.D. Mathur, and J.F. Scott, "A one-cent room-temperature magnetoelectric sensor," Nat. Mater., vol. 7, no. 2, pp. 93-94, 2008.
16. J. Ma, J. Hu, Z. Li, and C.W. Nan, "Recent progress in multiferroic magnetoelectric composites: from bulk to thin films," Adv. Mater., vol. 23, no. 9, pp. 1062-1087, 2011.
17. Y. Wang, J. Li, and D. Viehland, "Magnetoelectrics for magnetic sensor applications: status, challenges and perspectives," Mater. Today, vol. 17, no. 6, pp. 269-275, 2014.
18. M. Bibes and A. Barthélémy, "Multiferroics: towards a magnetoelectric memory," Nat. Mater., vol. 7, no. 6, pp. 425-426, 2008.
19. J.F. Scott, "Applications of magnetoelectrics," J. Mater. Chem., vol. 22, no. 11, pp. 4567-4574, 2012.
20. C.W. Nan, M.I. Bichurin, S. Dong, D. Viehland, and G. Srinivasan, "Multiferroic magnetoelectric composites: historical perspective, status, and future directions," J. Appl. Phys., vol. 103, no. 3, p. 031101, 2008.
21. H. Palneedi, V. Annapureddy, S. Priya, and J. Ryu, "Status and perspectives of multiferroic magnetoelectric composite materials and applications," Actuators, vol. 5, no. 1, p. 9, 2016.
22. L. Martin, Y. Chu, and R. Ramesh, "Advances in the growth and characterization of magnetic, ferroelectric, and multiferroic oxide thin films," Mater. Sci. Eng. R, vol. 68, no. 4-6, pp. 89-133, 2010.
23. S. Dong, J. Zhai, J. Li, D. Viehland, and S. Priya, "Multimodal system for harvesting magnetic and mechanical energy," Appl. Phys. Lett., vol. 93, no. 10, p. 103511, 2008.
24. H. Greve et al., "Giant magnetoelectric coefficients in (Fe₉₀Co₁₀)₇₈Si₁₂B₁₀-AlN thin film composites," Appl. Phys. Lett., vol. 96, no. 18, p. 182501, 2010.
25. Z. Chu et al., "Enhanced resonance magnetoelectric coupling in (1-1) connectivity composites," Adv. Mater., vol. 29, no. 19, p. 1606022, 2017.
26. J. Das, Y.Y. Song, N. Mo, P. Krivosik, and C.E. Patton, "Electric-field-tunable low loss multiferroic ferrimagnetic-ferroelectric heterostructures," Adv. Mater., vol. 21, no. 20, pp. 2045-2049, 2009.
27. P. Record, C. Popov, J. Fletcher, E. Abraham, Z. Huang, H. Chang, and R. Whatmore, "Direct and converse magnetoelectric effect in laminate bonded Terfenol-D-PZT composites," Sens. Actuators B Chem., vol. 126, no. 1, pp. 344-349, 2007.
28. M. Bichurin, V. Petrov, and G. Srinivasan, "Theory of low-frequency magnetoelectric coupling in magnetostrictive-piezoelectric bilayers," Phys. Rev. B, vol. 68, no. 5, p. 054402, 2003.
29. G. Srinivasan, E.T. Rasmussen, J. Gallegos, R. Srinivasan, Y.I. Bokhan, and V.M. Laletin, "Magnetoelectric bilayer and multilayer structures of magnetostrictive and piezoelectric oxides," Phys. Rev. B, vol. 64, no. 21, p. 214408, 2001.
30. S. Zhao, J.G. Wan, M. Yao, J.M. Liu, F.Q. Song, and G.H. Wang, "Flexible CoFe₂O₄-Bi₃.₁₅Nd₀.₈₅Ti₃O₁₂ thin films: integration of ferroelectric and magnetic properties," Adv. Mater., vol. 22, no. 21, pp. 2369-2373, 2010.
