Skip to main content
Log in

Structure and properties of 0.5Bi4Ti3O12-0.5BiFe0.98Mn0.02O3 films under different annealing atmospheres

  • Published:
Journal of Materials Science: Materials in Electronics Aims and scope Submit manuscript

Abstract

In this paper, 0.5Bi4Ti3O12–0.5BiFe0.98Mn0.02O3 (BTBF) films were prepared on FTO/glass substrates using the sol-gel method. The impacts of BTBF films on the grain structure, defect density, electrical properties and ageing properties were studied under air, oxygen and nitrogen-annealing atmospheres. X-ray diffraction (XRD) results demonstrate that the ferroelectric materials formed by the combination of Bi4Ti3O12 (BIT) and BiFe0.98Mn0.02O3 (BFMO) in the form of a solid solution show a bismuth-layered perovskite structure. X-ray photoelectron spectroscopy (XPS) shows that samples annealed under an O2 atmosphere have higher Fe3+: Fe2+ ratios and fewer oxygen vacancy defects. Meanwhile, the samples annealed under an O2 atmosphere show better ferroelectric properties (2Pr ≈ 22.0 µC/cm2) and a lower leakage current density (J ≈ 7.09 × 10− 6 A/cm2). In addition, the annealing atmosphere is also found to affect the light absorption performance of the samples, and the samples annealed under a N2 atmosphere show a smaller band gap and better light absorption performance. Finally, the ageing phenomenon for the samples is analysed, and the volumetric effect ageing mechanism is discussed.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

Data availability

All data generated or analyzed during this study are included in this article.

References

  1. J.P. Liu, Z.L. Lv, Y.X. Hou, L.P. Zhang, J.P. Cao, H.W. Wang, W.B. Zhao, C. Zhang, Y. Bai, K.K. Meng, X.G. Xu, J. Miao, Substantial reduction of leakage currents in La/Er/Zn/Ti multielement-doped BiFeO3 multiferroic thin films. Ceram. Int. 48, 17328–17334 (2022)

    Article  CAS  Google Scholar 

  2. R. Gao, Q. Zhang, Z. Xu, Z. Wang, W. Cai, G. Chen, X. Deng, X. Cao, X. Luo, C. Fu, Strong magnetoelectric coupling effect in BaTiO3@CoFe2O4 magnetoelectric multiferroic fluids. Nanoscale. 10, 11750–11759 (2018)

    Article  CAS  Google Scholar 

  3. W.J. Ma, Q. Sun, M.J. Sun, L. Bai, Y.Q. Liu, J.K. Zhang, J.H. Yang, Structural evolution-enabled BiFeO3 modulated by strontium doping with enhanced magnetic and photoelectric performance. Appl. Surf. Sci. 571, 151130 (2022)

    Article  CAS  Google Scholar 

  4. C.K. Wang, C. Xu, H.Y. Chen, X.X. Ma, Y.K. Chen, F. Chen, B.J. Kang, J.Y. Ge, W. Ren, S.X. Cao, Magnetoelectric phase diagram and magnetic field-induced reversal of electric polarization in Ba0.5Sr1.5Mg1.6Co0.4Fe12O22 single crystal. J. Alloys Compd. 886, 161266 (2021)

    Article  CAS  Google Scholar 

  5. R.L. Gao, Q.M. Zhang, Z.Y. Xu, Z.H. Wang, G. Chen, X.L. Deng, C.L. Fu, W. Cai, A comparative study on the structural, dielectric and multiferroic properties of Co0.6Cu0.3Zn0.1Fe2O4/Ba0.9Sr0.1Zr0.1Ti0.9O3 composite ceramics. Compos. Part B: Eng. 166, 204–212 (2019)

    Article  CAS  Google Scholar 

  6. L.H. Jin, M. Liu, C.H. Li, D.P. Song, B.B. Yang, X.B. Zhu, Evolution of structure and electrical properties of epitaxial BiFeO3 thin films through solution and annealing atmosphere. J. Alloys Compd. 843, 155910 (2020)

    Article  CAS  Google Scholar 

  7. L.Z. Zeng, Y.M. Lu, L.J. Zhang, X. Gong, J.F. Tang, G.N. Li, Structure, dielectric, and multiferroic properties of Bi0.85Nd0.15Fe0.98Zr0.02O3 in Ba and Ti co-doping. J. Mater. Sci.: Mater. Electron. 32, 18439–18449 (2021)

    CAS  Google Scholar 

  8. T.M. Pan, Y.C. Chou, J.L. Her, Effect of Yb-doping on structural and electrical properties of BiFeO3 thin films. Mater. Chem. Phys. 278, 125699 (2022)

    Article  CAS  Google Scholar 

  9. X.L. Liang, J.Q. Dai, C.C. Zhang, Effect of (Zn, Mn) co-doping on the structure and ferroelectric properties of BiFeO3 thin films. Ceram. Int. 48, 6347–6355 (2022)

    Article  CAS  Google Scholar 

  10. Y. Zhang, R.X. Huang, Z.H. Liang, F. Zhang, H.T. Lin, L.X. Lai, Y.J. Dai, Reduction inhibition of Fe3+ ions in Mn-doped 0.7BiFeO3-0.3BaTiO3 ceramics by direct reaction sintering. Ceram. Int. 48, 26696–26703 (2022)

    Article  CAS  Google Scholar 

  11. S.G. Huang, Q.N. Li, L. Yang, J.W. Xu, C.R. Zhou, G.H. Chen, C.L. Yuan, G.H. Rao, Enhanced piezoelectric properties by reducing leakage current in Co modified 0.7BiFeO3-0.3BaTiO3 ceramics. Ceram. Int. 44, 8955–8962 (2018)

    Article  CAS  Google Scholar 

  12. J.W. Liang, X.L. Zhu, L. Zhu, L. Liu, S.Y. Wu, X.Q. Liu, X.M. Chen, Magnetoelectric coupling in sm substituted 0.67BiFeO3- 0.33BaTiO3 ceramics. J. Alloys Compd. 901, 163681 (2022)

    Article  CAS  Google Scholar 

  13. C.H. Chen, J.L. Her, T.M. Pan, Structural properties of ferroelectric characteristics of mixed NiTiO3-BiFeO3 thin film by the sol-gel method. J. Phys. Chem. Sol. 152, 109986 (2021)

    Article  CAS  Google Scholar 

  14. C.B. Long, H.Q. Fan, W. Ren, J.Y. Zhao, Double polarization hysteresis and dramatic influence of small compositional variations on the electrical properties in Bi4Ti3O12 ceramics. J. Eur. Ceram. Soc. 39, 4103–4112 (2019)

    Article  CAS  Google Scholar 

  15. K. Shraddha, A.V. Badge, Deshpande, Effect of vanadium doping on structural, dielectric and ferroelectric properties of bismuth titanate (Bi4Ti3O12) ceramics. Ceram. Int. 45, 15307–15313 (2019)

    Article  Google Scholar 

  16. C. Lavado, M.G. Stachiotti, Fe3+/Nb5+ co-doping effects on the properties of Aurivillius Bi4Ti3O12 ceramics. J. Alloys Compd. 731, 914–919 (2018)

    Article  CAS  Google Scholar 

  17. R.X. Ti, F.Z. Huang, W.L. Zhu, J. He, T.T. Xu, C. Yue, J. Zhao, X.M. Lu, J.S. Zhu, Multiferroic and dielectric properties of Bi4LaTi3FeO15 ceramics. Ceram. Int. 41, S453–S457 (2015)

    Article  CAS  Google Scholar 

  18. D.P. Song, J. Yang, Y. Wang, Focus on the ferroelectric polarization behavior of four-layered Aurivillius multiferroic thin film. Ceram. Int. 45, 10080–10085 (2019)

    Article  CAS  Google Scholar 

  19. P.P. Jiang, X.L. Zhang, P. Chang, Z.G. Hu, W. Bai, Y.W. Li, J.H. Chu, Spin-phonon interactions of multiferroic Bi4Ti3O12-BiFeO3 ceramics: low-temperature Raman scattering and infrared reflectance spectra investigations. J. Appl. Phys. 115, 144101 (2014)

    Article  Google Scholar 

  20. Y.H. Zhao, B. Yang, Y.P. Liu, Y.P. Zhou, Q. Wu, S.F. Zhao, Capturing carriers and driving depolarization by defect Engineering for Dielectric Energy Storage. ACS Appl. Mater. Interfaces 14, 6547–6559 (2022)

    Article  CAS  Google Scholar 

  21. Y.P. Zhou, J.Y. Chen, B. Yang, S.F. Zhao, Ultrahigh energy storage performances derived from the relaxation behaviors and inhibition of the grain growth in La doped Bi5Ti3FeO15 films. Chem. Eng. J. 424, 130435 (2021)

    Article  CAS  Google Scholar 

  22. Z.H. Tang, J.Y. Chen, B. Yang, S.F. Zhao, Energy storage performances regulated by layer selection engineering for doping in multi-layered perovskite relaxor ferroelectric films. Appl. Phys. Lett. 114, 163901 (2019)

    Article  Google Scholar 

  23. C. Feng, C.H. Yang, F.J. Geng, P.P. Lv, Q. Yao, Microstructure and electrical properties mediated by defects in Na0.5Bi0.5Ti0.98Mn0.02O3 thin film under different annealing atmospheres. J. Eur. Ceram. Soc. 36, 527–532 (2016)

    Article  CAS  Google Scholar 

  24. M. Shi, E.Y. Men, Y.D. Xu, R.Z. Zuo, L. Guo, Z.L. Si, K.Z. Hu, H. Chen, Tiancheng Bai, Bi3.4Eu0.6Ti3O12/Ni0.7Cu0.3Fe2O4 films annealed under different atmosphere with enhanced magnetoelectric coupling effect. Ceram. Int. 48, 2406–2414 (2022)

    Article  CAS  Google Scholar 

  25. L. Jin, M. Liu, C. Li, D. Song, B. Yang, X. Zhu, Evolution of structure and electrical properties of epitaxial BiFeO3 thin films through solution and annealing atmosphere. J. Alloys Compd. 843, 155910 (2020)

    Article  CAS  Google Scholar 

  26. H.Z. Chen, M.C. Kao, S.L. Young, C.C. Yu, C.H. Lin, C.M. Lee, C.R. Ou, Effects of annealing atmosphere on microstructure and ferroelectric properties of praseodymium-doped Bi4Ti3O12 thin films prepared by sol–gel method. Thin Solid Films. 517, 4818–4821 (2009)

    Article  CAS  Google Scholar 

  27. Y.P. Liu, F. Guo, B. Yang, S.F. Zhao, Enhanced photovoltaic effect derived from the regulation of Jahn-Teller distortion in a lattice compensation structure. Appl. Phys. Lett. 119, 233901 (2021)

    Article  CAS  Google Scholar 

  28. X.F. Zhao, H.Y. Liu, X.Y. Pan, L.X. Wang, Z. Feng, Z.B. Ma, F.Q. Zhang, L.Y. Zhu, Q.B. Tian, S.H. Fan, Study on properties of BiFe0.98Mn0.02O3/Sr2Bi4Ti5O18 double-layer composite films. J. Alloys Compd. 836, 155433 (2020)

    Article  CAS  Google Scholar 

  29. S.J. Yang, F.Q. Zhang, X.B. Xie, H.J. Sun, L.P. Zhang, S.H. Fan, Effects of precursor concentration on electric properties of BiFe0.98Mn0.02O3 thin films prepared by sol–gel method. J. Sol-Gel Sci. Technol. 85, 158–165 (2017)

    Article  Google Scholar 

  30. Y. Liu, Z.B. Ma, Y.Y. Wang, B.D. Yao, J.X. He, J. Li, F.Q. Zhang, Effect of annealing temperature on the properties of 0.5Bi4Ti3O12-0.5BiFe0.98Mn0.02O3 thin films. Ceram. Int. 48, 28112–28120 (2022)

    Article  CAS  Google Scholar 

  31. Y.Y. Wang, Z.Y. Li, Z.B. Ma, L.X. Wang, X.D. Guo, Y. Liu, B.D. Yao, F.Q. Zhang, L.Y. Zhu, Phase structure and Electrical Properties of Sm-Doped BiFe0.98Mn0.02O3 thin Films. Nanomaterials (Basel) 12, 108 (2021)

    Article  Google Scholar 

  32. J. Li, N. Sha, Z. Zhao, Effect of annealing atmosphere on the ferroelectric properties of inkjet printed BiFeO3 thin films. Appl. Surf. Sci. 454, 233–238 (2018)

    Article  CAS  Google Scholar 

  33. S.J. Sun, W.Y. Wang, J.Q. Chen, Z.Y. Xiao, N. Cheng, Z.Q. Zhao, Y.S. Tian, X.F. Yin, Substrate- and layer-effects on structural and photovoltaic properties of spin-coated Aurivillius-type Bim+1Fem–3Ti3O3m + 3 thin films. J. Alloys Compd. 851, 156833–156839 (2021)

    Article  CAS  Google Scholar 

  34. Y.W. Lu, X.D. Qi, Hydrothermal synthesis of pure and Sb-doped BiFeO3 with the typical hysteresis loops of ideal ferroelectrics. J. Alloys Compd. 774, 386–395 (2019)

    Article  CAS  Google Scholar 

  35. Y.Y. Wang, Z.Y. Li, Z.B. Ma, L.X. Wang, X.D. Guo, Y. Liu, B.D. Yao, F.Q. Zhang, L.Y. Zhu, Phase structure and Electrical Properties of Sm-Doped BiFe0. 98Mn0. 02O3 thin Films. Nanomaterials. 12(1), 108 (2021)

    Article  Google Scholar 

  36. Z.B. Ma, H.Y. Liu, L.X. Wang, B.D. Yao, Y.Y. Wang, Y. Liu, F.Q. Zhang, W.W. Qin, J. Xu, Modified ferroelectric and photovoltaic properties of BiFe0.91Zr0.09O3 thin films via altered annealing atmospheres. J. Mater. Chem. C 9, 14659–14668 (2021)

    Article  CAS  Google Scholar 

  37. X. Deng, Z. Zeng, R. Xu, X. Qin, X. Li, Y. Wang, R. Gao, Z. Wang, G. Chen, W. Cai, C. Fu, Effect of annealing atmosphere on structural and multiferroic properties of BiFeO3 thin film prepared by RF magnetron sputtering. J. Mater. Sci.: Mater. Electron. 30, 16502–16509 (2019)

    CAS  Google Scholar 

  38. J.X. Wang, L. Luo, C.L. Han, R. Yun, X.G. Tang, Y.J. Zhu, Z.G. Nie, W.R. Zhao, Z.C. Feng, The microstructure, Electric, Optical and Photovoltaic Properties of BiFeO3 Thin Films prepared by Low Temperature Sol-Gel Method. Mater. (Basel) 12, 1444 (2019)

    Article  CAS  Google Scholar 

  39. Z.B. Ma, H.Y. Liu, L.X. Wang, F.Q. Zhang, L.Y. Zhu, S.H. Fan, Phase transition and multiferroic properties of Zr-doped BiFeO3 thin films. J. Mater. Chem. C 8, 17307–17317 (2020)

    Article  CAS  Google Scholar 

  40. J.G. Wu, J. Wang, D.Q. Xiao, J.G. Zhu, Leakage mechanism of cation -modified BiFeO3 thin film. AIP Adv. 1, 022138 (2011)

    Article  Google Scholar 

  41. P.M. Raj, B.W. Lee, D. Balaraman, R.R. Tummala, Leakage current analysis of hydrothermal BaTiO3 thin films. J. Electroceram. 27, 169–175 (2011)

    Article  CAS  Google Scholar 

  42. F. Yang, F.W. Zhang, G.D. Hu, Z.H. Zong, M.H. Tang, Thickness-dependent ferroelectric behavior of predominantly (117)-oriented Bi3.15Nd0.85Ti3O12 thin-film capacitors. Appl. Phys. Lett. 106, 172903 (2015)

    Article  Google Scholar 

  43. K. Yamaguchi, M. Gomi, Y. Shimizu, T. Yokota, Sputter-epitaxy and electric properties of multiferroic Bim+1Fem–3Ti3O3m + 3 thin films. Thin Solid Films 519, 8330–8333 (2011)

    Article  CAS  Google Scholar 

  44. Y.J. Ou, J.Q. Shi, Q.Q. Yan, C.L. Li, Y. Zheng, Ethanol-assisted molten salt synthesis of Bi4Ti3O12/Bi2Ti2O7 with enhanced visible light photocatalytic performance. Inorg. Chem. Commun. 133, 108867 (2021)

    Article  CAS  Google Scholar 

  45. Y.M. Huang, Y. Yu, Y.F. Yu, B. Zhang, Oxygen Vacancy Engineering in Photocatalysis. Solar RRL 4, 2000037 (2020)

    Article  CAS  Google Scholar 

  46. Z.Y. Li, Y.S. Xie, Y.F. Wang, Y. Peng, Z.Z. Deng, B.X. Liu, G.H. Zhang, X.Q. Wang, F.Q. Zhang, L.Y. Zhu, Fabrication, characterization and application of single-phase hollow BiFeO3 nanofibers as an efficient visible-light photocatalyst for degradation of rhodamine B in wastewater. J. Solid State Chem. 317, 123707 (2023)

    Article  CAS  Google Scholar 

  47. F.L. Wang, A. Jain, Y. Li, N. Wang, Y.L. Lu, L. Zhu, Y.G. Wang, F.G. Chen, Enhanced magnetic, ferroelectric, and photocatalytic properties of (1-x)BiFeO3-xBaTiO3 (0.0 ≤ x ≤ 0.4) powders,. Ceram. Int. 46, 16416–16421 (2020)

    Article  CAS  Google Scholar 

  48. C.H. Yang, J.Q. Sun, Z.D. Yi, Y.Y. Yao, X.S. Sun, Comparative study on dielectric behavior in fresh and aged Na0.5Bi0.5 (Ti, Fe, W) O3 thin films  Ceram. Int. 43, 7690–7694 (2017)

    Article  CAS  Google Scholar 

  49. F.Q. Zhang, P. Shen, H.Y. Liu, L.X. Wang, X.D. Guo, X.F. Zhao, Z.B. Ma, Q.B. Tian, S.H. Fan, Effects of the annealing atmosphere on the microstructure and properties of BiFe0.99Zn0.01O3 films. Ceram. Int. 46, 4314–4321 (2020)

    Article  CAS  Google Scholar 

  50. H.Y. Liu, L.X. Wang, F.Q. Zhang, X.D. Guo, P. Shen, X.F. Zhao, S.H. Fan, The effect of the annealing atmosphere on the properties of Sr2Bi4Ti5O18 ferroelectric thin films. Ceram. Int. 45, 18320–18326 (2019)

    Article  CAS  Google Scholar 

  51. X. Ren, Large electric-field-induced strain in ferroelectric crystals by point-defect-mediated reversible domain switching. Nat. Mater. 3, 91–94 (2004)

    Article  CAS  Google Scholar 

  52. P.P. Lv, C.H. Yang, F.J. Geng, C. Feng, X.M. Jiang, G.D. Hu, Effect of defect dipole-induced aging on the dielectric property of Fe3+-doped Na0.5Bi0.5TiO3 thin film. Ceram. Int. 42, 2876–2881 (2016)

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by Shandong Provincial Natural Science Fund (ZR2022ME071), the Program of the Housing and Urban-Rural Construction Department of Shandong Province (2019-K7-10) and State Key Laboratory of Silicate Materials for Architectures (Wuhan University of Technology) (SYSJJ2020-05).

Author information

Authors and Affiliations

Authors

Contributions

YL: prepared the BTBF films and performed all measurements. FQZ and JL: supervised the experiments and suggested changes to the paper. YYW, GDW, BDY and JXH: contributed to the revision of the manuscript and collation of experimental data. All authors discussed the results and commented on the manuscript. All authors have given approval to the final version of the manuscript.

Corresponding author

Correspondence to Fengqing Zhang.

Ethics declarations

Conflict of interest

The authors declare that they have no competing financial interests.

Additional information

Publisher’s Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Liu, Y., Wang, Y., Wang, G. et al. Structure and properties of 0.5Bi4Ti3O12-0.5BiFe0.98Mn0.02O3 films under different annealing atmospheres. J Mater Sci: Mater Electron 34, 364 (2023). https://doi.org/10.1007/s10854-022-09735-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s10854-022-09735-z

Navigation