Abstract
Barium titanate (BaTiO3) phase is observed in thin films synthesized via an electroless chemical bath deposition (CBD) method. Solution molarity is varied as 0.1–1.2 M. Temperature of solution is kept at 78 °C under continuous stirring. XRD analyses show formation of tetragonal dominant phase of BaTiO3 along with titania peaks at low molarity values, whereas tetragonal BaTiO3 is observed at higher molarity values. Optical results show maximum transmission (∼80%) for 1.2 M-based annealed thin films. Variation in direct band gap is observed from ∼3.9 to 4.6 eV in case of annealed thin films. High value of dielectric constant (~ 530 at log f = 3) and low value of tangent loss is attained for thin films prepared with 1.2 M. The frequency-dependent dielectric behavior is attained for BaTiO3. Temperature-dependent dielectric study shows effect of grains and grain boundaries. FTIR analyses show the formation of tetragonal barium titanate band. Maximum spontaneous polarization (~ 6 × 10−3 μC/cm2) and remnant polarization (~ 2 × 10−3 μC/cm2) along with maximum efficiency are observed for the sample prepared with 1.2 M solution. It is worth-mentioning here that frequency dependent dielectric constant along with ferroelectric properties of BaTiO3 are observed in the present work making this material potential candidate for multilayer capacitor-based applications.
Graphical abstract
Similar content being viewed by others
Data availability
Relevant data has been used in the manuscript.
References
D. Hu, Z. Pan, X. Tan, F. Yang, J. Ding, X. Zhang, P. Li, J. Liu, J. Zhai, H. Pan, Optimization the energy density and efficiency of BaTiO3-based ceramics for capacitor applications. Chem. Eng. J. 409, 127375 (2021)
Li, D., Lin, Y., Zhang, M., & Yang, H. (2020). Achieved ultrahigh energy storage properties and outstanding charge–discharge performances in (Na0. 5Bi0. 5) 0.7 Sr0. 3TiO3-based ceramics by introducing a linear additive. Chemical Engineering Journal, 392, 123729.
W.B. Li, D. Zhou, W.F. Liu, J.Z. Su, F. Hussain, D.W. Wang, G. Wang, Z.L. Lu, Q.P. Wang, High-temperature BaTiO3-based ternary dielectric multilayers for energy storage applications with high efficiency. Chem. Eng. J. 414, 128760 (2021)
J. Wang, S. Jiang, D. Jiang, J. Tian, Y. Li, Y. Wang, Microstructural design of BaTiO3-based ceramics for temperature-stable multilayer ceramic capacitors. Ceram. Int. 38(7), 5853–5857 (2012)
K. Hong, T.H. Lee, J.M. Suh, S.H. Yoon, H.W. Jang, Perspectives and challenges in multilayer ceramic capacitors for next generation electronics. J. Mater. Chem. C 7(32), 9782–9802 (2019)
G. Tanvir, M. Saleem, H. Jabbar, A. Hamza, M.A. Hussain, M.Z. Khan, A.H. Baluch, M. Irfan, M.S. Butt, F. Naeem, A. Ghaffar, A. Maqbool, Study of ferroelectric and piezoelectric response of heat-treated surfactant-based BaTiO3 nanopowder for high energy capacitors. Mater. Sci. Eng. B 287, 116100 (2023)
Xiao, D. Q., Wu, J. G., Wu, L., Zhu, J. G., Yu, P., Lin, D. M., ... & Sun, Y. (2009). Investigation on the composition design and properties study of perovskite lead-free piezoelectric ceramics. Journal of materials science, 44, 5408–5419.
Wu, H., & Zhu, X. (2016). Perovskite oxide nanocrystals-synthesis, characterization, functionalization, and novel applications. Perovskite Materials-Synthesis, Characterisation, Properties, and Applications; Pan, L., Zhu, G., Eds, 153–183.
J.M. Hwu, W.H. Yu, W.C. Yang, Y.W. Chen, Y.Y. Chou, Characterization of dielectric barium titanate powders prepared by homogeneous precipitation chemical reaction for embedded capacitor applications. Mater. Res. Bull. 40(10), 1662–1679 (2005)
Saravanan, R. (2018). Titanate based ceramic dielectric materials. Materials Research Forum LLC.
Rahman, M. A. (2023). Understanding of doping sites and versatile applications of heteroatom modified BaTiO3 ceramic. Journal of Asian Ceramic Societies, 1–10.
S. Mtougui, R. Khalladi, S. Ziti, H. Labrim, L. Bahmad, Magnetic properties of the perovskite BiFeO3: Monte Carlo simulation. Superlattices Microstruct. Microstruct. 123, 111–118 (2018)
A. Navrotsky, Energetics and crystal chemical systematics among ilmenite, lithium niobate, and perovskite structures. Chem. Mater. 10(10), 2787–2793 (1998)
Pola, S., Panwar, N., & Coondoo, I. (2021). Perovskite and Piezoelectric Materials. BoD–Books on Demand.
V. Buscaglia, C.A. Randall, Size and scaling effects in barium titanate. An overview. J. Eur. Ceram. Soc. 40, 3744–3758 (2020)
W.D. Nothwang, M.W. Cole, S.G. Hirsch, Grain growth and residual stress in BST thin films. Integr. Ferroelectr.. Ferroelectr. 71(1), 107–113 (2005)
A. Karvounis, F. Timpu, V.V. Vogler-Neuling, R. Savo, R. Grange, Barium titanate nanostructures and thin films for photonics. Advanced Optical Materials 8(24), 2001249 (2020)
H. Huang, X. Yao, Preparation of BaTiO3 thin films by mist plasma evaporation on MgO buffer layer. Ceram. Int. 30(7), 1535–1538 (2004)
A. Ianculescu, B. Despax, V. Bley, T. Lebey, R. Gavrilă, N. Drăgan, Structure–properties correlations for barium titanate thin films obtained by rf-sputtering. J. Eur. Ceram. Soc. 27(2–3), 1129–1135 (2007)
C.K. Tan, G.K. Goh, Growth and dielectric properties of solvothermal BaTiO3 polycrystalline thin films. Thin Solid Films 515(16), 6572–6576 (2007)
C.K. Tan, G.K.L. Goh, G.K. Lau, Growth and dielectric properties of BaTiO3 thin films prepared by the microwave-hydrothermal method. Thin Solid Films 516(16), 5545–5550 (2008)
Y. Huang, J. Lin, H. Du, L. Gao, Y. Hu, Preparation and photoluminescence properties of ZnO/amorphous-BaTiO3 thin-films by sol–gel process. Mater. Lett. 60(29–30), 3818–3821 (2006)
O. Harizanov, A. Harizanova, T. Ivanova, Formation and characterization of sol–gel barium titanate. Mater. Sci. Eng. B 106(2), 191–195 (2004)
F.M. Pontes, C.D. Pinheiro, E. Longo, E.R. Leite, S.R. De Lazaro, R. Magnani, P.S. Pizani, T.M. Boschi, F. Lanciotti, Theoretical and experimental study on the photoluminescence in BaTiO3 amorphous thin films prepared by the chemical route. J. Lumin.Lumin. 104(3), 175–185 (2003)
L. Singh, R. Singh, Effect of dopant concentration on structural properties of chemical bath deposited Mn-doped Pbs nanocrystalline thin films. Chalcogenide Letters 17(7), 375–384 (2020)
S. Khan, N. Humera, S. Niaz, S. Riaz, S. Atiq, S. Naseem, Simultaneous normal–Anomalous dielectric dispersion and room temperature ferroelectricity in CBD perovskite BaTiO3 thin films. J. Market. Res. 9(5), 11439–11452 (2020)
S.S. Kumbhar, M.A. Mahadik, P.K. Chougule, V.S. Mohite, Y.M. Hunge, K.Y. Rajpure, A.V. Moholkar, C.H. Bhosale, Structural and electrical properties of barium titanate (BaTiO3) thin films obtained by spray pyrolysis method. Mater. Sci.-Pol. 33(4), 852–861 (2015)
F. He, W. Ren, G. Liang, P. Shi, X. Wu, X. Chen, Structure and dielectric properties of barium titanate thin films for capacitor applications. Ceram. Int. 39, S481–S485 (2013)
B. Bajac, J. Vukmirovic, D. Tripkovic, E. Djurdjic, J. Stanojev, Ž Cvejic, B. Škoric, V.V. Srdic, Structural characterization and dielectric properties of BaTiO3 thin films obtained by spin coating. Process. Appl. Ceramics 8(4), 219–224 (2014)
Y. Gao, M. Yuan, X. Sun, J. Ouyang, In situ preparation of high quality BaTiO3 dielectric films on Si at 350–500 C. J. Mater. Sci. 28(1), 337–343 (2017)
Schumann, T., Zhu, X., Neff, J., Hebard, A., Zmuda, H., & Yoon, Y. K. (2018). Solely Calcine Controlled Ferroelectricity and Resistivity of Barium Titanate Thin Films and Their Advanced Memory Applications. In 2018 IEEE 68th Electronic Components and Technology Conference (ECTC), 1402–1406.
M. Tahir, S. Riaz, U. Khan, S.S. Hussain, A. Nairan, A. Akbar, S. Naseem, Enhanced structural and magnetic ordering in as-synthesized Ca doped bismuth iron oxide nanoceramics. J. Alloy. Compd. 832, 154725 (2020)
Pan, L., & Zhu, G. (2016). Perovskite materials: synthesis, characterisation, properties, and applications. BoD–Books on Demand.
M. Guo, G. Wang, Y. Zhao, H. Li, K. Tang, Y. Zhao, K. Burgess, Preparation of Nano-ZrO2 powder via a microwave-assisted hydrothermal method. Ceram. Int. 47(9), 12425–12432 (2021)
I. Sanaullah, H.N. Khan, A. Sajjad, S. Khan, A.N. Sabri, S. Naseem, S. Riaz, Improved osteointegration response using high strength perovskite BaTiO3 coatings prepared by chemical bath deposition. J. Mech. Behav. Biomed. Mater.Behav. Biomed. Mater. 138, 105635 (2023)
H.P. Klug, L.E. Alexander, X-ray Diffraction Procedures for Polycrystalline and Amorphous Materials (Wiley, New York, 1974)
V.V. Deshmane, A.V. Patil, Effects of additives on structural and magnetic properties of iron oxide. Int. J. Nanosci.Nanosci. 19(04), 1950025 (2020)
S. Riaz, S. Naseem, Effect of reaction temperature and time on the structural properties of Cu (In, Ga) Se2 thin films deposited by sequential elemental layer technique. J Mater Sci Technol-Shenyang 23(4), 499 (2007)
L. Xu, G. Zheng, J. Miao, F. Xian, Dependence of structural and optical properties of sol–gel derived ZnO thin films on sol concentration. Appl. Surf. Sci. 258(19), 7760–7765 (2012)
G. Madras, B.J. McCoy, Transition from nucleation and growth to Ostwald ripening. Chem. Eng. Sci. 57(18), 3809–3818 (2002)
A. Awan, M. Nadeem, S. Riaz, S.S. Hussain, F. Majid, S. Naseem, Molarity dependent oscillatory structural and magnetic behavior of phase pure BiFeO3 thin films: sol–gel approach. Ceram. Int. 45(4), 5111–5123 (2019)
G. Arandhara, J. Bora, P.K. Saikia, Effect of pH on the crystallite size, elastic properties and morphology of nanostructured ZnS thin films prepared by chemical bath deposition technique. Mater. Chem. Phys. 241, 122277 (2020)
A. Moghtada, R. Ashiri, Enhancing the formation of tetragonal phase in perovskite nanocrystals using an ultrasound assisted wet chemical method. Ultrason. Sonochem.. Sonochem. 33, 141–149 (2016)
Rabe, K. M., Ahn, C. H., & Triscone, J. M. (Eds.). (2007). Physics of ferroelectrics: a modern perspective (Vol. 105). Springer Science & Business Media; Usher, T. M., Kavey, B., Caruntu, G., & Page, K. (2020). Effect of BaCO3 impurities on the structure of BaTiO3 nanocrystals: implications for multilayer ceramic capacitors. ACS Applied Nano Materials, 3(10), 9715–9723.
T. Ishii, H. Wakita, K. Ogasawara, Y.S. Kim, The DV-Xα molecular-orbital calculation method. Springer International Publishing. (2015)
M. Weller, M.T. Weller, T. Overton, J. Rourke, F. Armstrong, Inorganic chemistry (Oxford University Press, USA, 2014)
B. Kaufmann, P. Christen, Recent extraction techniques for natural products: microwave-assisted extraction and pressurised solvent extraction. Phytochem. Anal.. Anal. 13(2), 105–113 (2002)
V. Kaushik, V. Kumar, D. Kumar, R. Kumar, V. Singh, M. Kumar, S.K. Sharma, Effect of aging on microstructural and optical properties of sol-gel dip coated BaTiO3 thin films. Appl. Surface Sci. Adv. 16, 100418 (2023)
S. Halder, T. Schneller, R. Waser, S.B. Majumder, Electrical and optical properties of chemical solution deposited barium hafnate titanate thin films. Thin Solid Films 516(15), 4970–4976 (2008)
Fox, M. (2002). Optical properties of solids.
C.E. Kim, P. Moon, S. Kim, J.M. Myoung, H.W. Jang, J. Bang, I. Yun, Effect of carrier concentration on optical bandgap shift in ZnO: Ga thin films. Thin Solid Films 518(22), 6304–6307 (2010)
B.E. Sernelius, K.F. Berggren, Z.C. Jin, I. Hamberg, C.G. Granqvist, Band-gap tailoring of ZnO by means of heavy Al doping. Phys. Rev. B 37(17), 10244 (1988)
E.K. Barimah, A. Boontan, D.P. Steenson, G. Jose, Infrared optical properties modulation of VO2 thin film fabricated by ultrafast pulsed laser deposition for thermochromic smart window applications. Sci. Rep. 12(1), 11421 (2022)
S. Riaz, M. Abutalib, S. Naseem, Structural, optical, and dielectric properties of aluminum oxide nanofibers synthesized by a lower-temperature sol-gel approach. J. Electron. Mater. 45(10), 5185–5197 (2016)
A.A. Aboud, A. Mukherjee, N. Revaprasadu, A.N. Mohamed, The effect of Cu-doping on CdS thin films deposited by the spray pyrolysis technique. J. Market. Res. 8(2), 2021–2030 (2019)
Jandow, N. N., Habubi, N. F., Al-Baidhany, I. A., & Qaeed, M. A. (2019). Annealing Effects on Band Tail Width, Urbach Energy and Optical Parameters of Fe2O3: Ni Thin Films Prepared by Chemical Spray Pyrolysis Technique. International Journal of Nanoelectronics & Materials, 12(1).
A.S. Hassanien, A.A. Akl, Effect of Se addition on optical and electrical properties of chalcogenide CdSSe thin films. Superlattices Microstruct. Microstruct. 89, 153–169 (2016)
Barsoukov, E., & Macdonald, J. R. (2005). Impedance Spectroscopy Theory, Experiment, and Applications. (Ed. 2nd). John Wiley &Sons, 595.
N. Kumari, V. Kumar, S.K. Singh, Synthesis, structural and dielectric properties of Cr3+ substituted Fe3O4 nano-particles. Ceram. Int. 40(8), 12199–12205 (2014)
C.G. Koops, On the dispersion of resistivity and dielectric constant of some semiconductors at audiofrequencies. Phys. Rev. 83(1), 121 (1951)
Y.F. Cui, Y.G. Zhao, L.B. Luo, J.J. Yang, H. Chang, M.H. Zhu, T.L. Ren, Dielectric, magnetic, and magnetoelectric properties of La and Ti codoped BiFeO 3. Appl. Phys. Lett. 97(22), 222904 (2010)
R. Gao, Q. Zhang, Z. Xu, Z. Wang, G. Chen, X. Deng, C. 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. B Eng. 166, 204–212 (2019)
F. Hcini, S. Hcini, M.A. Wederni, B. Alzahrani, H. Al Robei, K. Khirouni, S. Zemni, M.L. Bouazizi, Structural, optical, and dielectric properties for Mg0· 6Cu0· 2Ni0· 2Cr2O4 chromite spinel. Physica B B 624, 413439 (2022)
R. Gao, Z. Wang, G. Chen, X. Deng, W. Cai, C. Fu, Influence of core size on the multiferroic properties of CoFe2O4@ BaTiO3 core shell structured composites. Ceram. Int. 44, S84–S87 (2018)
Y. Gao, J. Wang, L. Wu, S. Bao, Y. Shen, Y. Lin, C. Nan, Tunable magnetic and electrical behaviors in perovskite oxides by oxygen octahedral tilting. Sci. China Mater. 58(4), 302–312 (2015)
C. Yang, J.S. Jiang, F.Z. Qian, D.M. Jiang, C.M. Wang, W.G. Zhang, Effect of Ba doping on magnetic and dielectric properties of nanocrystalline BiFeO3 at room temperature. J. Alloy. Compd. 507(1), 29–32 (2010)
Verma, K. C., Ram, M., Singh, J., & Kotnala, R. K. (2011). Impedance spectroscopy and dielectric properties of Ce and La substituted Pb0.7Sr0.3 (Fe0.012Ti0.988) O3 nanoparticles. Journal of Alloys and Compounds, 509(15), 4967–4971.
R. Gao, X. Qin, Q. Zhang, Z. Xu, Z. Wang, C. Fu, G. Chen, X. Deng, W. Cai, Enhancement of magnetoelectric properties of (1–x) Mn0. 5Zn0. 5Fe2O4-xBa0. 85Sr0. 15Ti0. 9Hf0. 1O3 composite ceramics. J. Alloy. Compd. 795, 501–512 (2019)
S. Khan, S. Riaz, F. Arshad, M. Azhar, N. Ahmad, H. Noor, S. Atiq, S. Naseem, Role of Ca doping on oxygen vacancy production in modulating dielectric, ferroelectric and magnetic polarization in BaTiO3 thin films. J. Market. Res. 16, 993–1007 (2022)
Sharma, G., Kumar, A., & Dhiman, P. (2021). Ferrite: Nanostructures with Tunable Properties and Diverse Applications. (Vol 112). Materials Research Forum LLC, 378.
M.D. Hossain, M.N.I. Khan, A. Nahar, M.A. Ali, M.A. Matin, S.M. Hoque, A.T.M.K. Jamil, Tailoring the properties of Ni-Zn-Co ferrites by Gd3+ substitution. J. Magn. Magn. Mater.Magn. Magn. Mater. 497, 165978 (2020)
S. Khalid, S. Riaz, S. Naeem, A. Akbar, S.S. Hussain, Y.B. Xu, S. Naseem, Spin polarization and magneto-dielectric coupling in Al-modified thin iron oxide films-microwave mediated sol-gel approach. J. Ind. Eng. Chem. 103, 49–66 (2021)
S.B. Bukhari, M. Imran, M. Bashir, S. Riaz, S. Naseem, Room temperature stabilized TiO2 doped ZrO2 thin films for teeth coatings–A sol-gel approach. J. Alloy. Compd. 767, 1238–1252 (2018)
K. Pubby, K.V. Babu, S.B. Narang, Magnetic, elastic, dielectric, microwave absorption and optical characterization of cobalt-substituted nickel spinel ferrites. Mater. Sci. Eng. B 255, 114513 (2020)
Waqas, M., Niaz, S., Batoo, K. M., Khalid, S., Atiq, S., Xu, Y. B., Naseem, S., & Riaz, S. (2023). Robust Ferromagnetism and Magneto-Dielectric Anomalies in (Al, Cr) co-doped Iron Oxide Thin Films-Microwave Mediated Sol-Gel Approach. Journal of Materials Research and Technology.
TD charge carriers] Kumar, P., Kumar, P., Kumar, A., Meena, R. C., Tomar, R., Chand, F., & Asokan, K. (2016). Structural, morphological, electrical and dielectric properties of Mn doped CeO2. Journal of Alloys and Compounds, 672, 543-548
Ben, L., & Sinclair, D. C. (2011). Anomalous Curie temperature behavior of A-site Gd-doped BaTiO3 ceramics: The influence of strain. Applied Physics Letters, 98(9).
T. Walther, N. Quandt, R. Köferstein, R. Roth, M. Steimecke, S.G. Ebbinghaus, BaTiO3–CoFe2O4–BaTiO3 trilayer composite thin films prepared by chemical solution deposition. J. Eur. Ceram. Soc. 36(3), 559–565 (2016)
Caruta, B. M. (2006). Trends in materials science research. Nova Publishers.
M. Singh, B.C. Yadav, A. Ranjan, M. Kaur, S.K. Gupta, Synthesis and characterization of perovskite barium titanate thin film and its application as LPG sensor. Sens. Actuators, B Chem. 241, 1170–1178 (2017)
A. Abdel Aal, T. Hammad, M. Zawrah, I. Battisha, A. AbouHammad, FTIR study of nanostructure perovskite BaTiO3 doped with both Fe^3+ and Ni^2+ Ions prepared by sol-gel technique. Acta Phys. Pol., A 126(6), 1318–1321 (2014)
M.E. Lines, A.M. Glass, Principles and applications of ferroelectrics and related materials (Oxford University Press, 2001)
R. Thomas, V.K. Varadan, S. Komarneni, D.C. Dube, Diffuse phase transitions, electrical conduction, and low temperature dielectric properties of sol–gel derived ferroelectric barium titanate thin films. J. Appl. Phys. 90(3), 1480–1488 (2001)
Acknowledgements
The authors are thankful to Higher Education Commission and Punjab University for the financial support. The author K M Batoo would like to thank Researchers Supporting Project No. (RSP2024R148), King Saud University, Riyadh, Saudi Arabia for the financial support.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
Authors declare no conflict of interests.
Supplementary Information
Below is the link to the electronic supplementary material.
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.
About this article
Cite this article
Azhar, M., Niaz, S., Batoo, K.M. et al. Stirring-mediated dielectric and ferroelectric response in perovskite BaTiO3 for multilayer capacitor applications. J. Korean Ceram. Soc. (2024). https://doi.org/10.1007/s43207-024-00370-4
Received:
Revised:
Accepted:
Published:
DOI: https://doi.org/10.1007/s43207-024-00370-4