Abstract
Ba0.85Ca0.15Zr0.1Ti0.9O3 (BCZT) ferroelectric epitaxial films deposited at different oxygen partial pressure were successfully obtained by pulsed laser deposition. The effects of oxygen partial pressure on the phase structure, microstructure, electrical properties and leakage mechanism were studied. The results showed that the BCZT epitaxial films have a smooth surface, uniform thickness, well integrated with substrate and no elemental segregation. BCZT epitaxial film with oxygen partial pressure of 15 Pa exhibited the optimal electrical properties (2Pr–22.48 µC/cm2, Jleak ∼ 1.42 × 10−3 A/cm2). The results of conduction mechanism fitting indicated that BCZT film conductivity mechanism followed the Ohmic mechanism at low electric fields, while it followed the Fowler–Nordheim tunneling mechanism at high electric fields.
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References
R. Soleimanzadeh, M. Kolahdouz, P. Ebrahimi, M. Norouzi, H. Aghababa, H. Radamson, Ultra-high efficiency piezotronic sensing using piezo-engineered FETs. Sens. Actuat A-Phys. 270, 240–244 (2018)
R. Guo, L.E. Cross, S.E. Park, B. Noheda, D.E. Cox, G. Shirane, Origin of the high piezoelectric response in PbZr1−xTixO3. Phys. Rev. Lett. 84, 5423–5426 (2000)
B. Noheda, J.A. Gonzalo, L.E. Cross, R. Guo, S.E. Park, D.E. Cox, G. Shirane, Tetragonal-to-monoclinic phase transition in a ferroelectric perovskite: the structure of PbZr0.52Ti0.48O3. Phys. Rev. B 61, 8687–8695 (2000)
M.D. Maeder, D. Damjanovic, N. Setter, Lead free piezoelectric materials. J. Electroceram. 13, 385–392 (2004)
S.T. Zhang, A.B. Kounga, E. Aulbach, H. Ehrenberg, J. Rodel, Giant strain in lead-free piezoceramics Bi0.5Na0.5TiO3–BaTiO3–K0.5Na0.5NbO3 system. Appl. Phys. Lett. 91, 112906 (2007)
J. Rodel, K.G. Webber, R. Dittmer, W. Jo, M. Kimura, D. Damjanovic, Transferring lead-free piezoelectric ceramics into application. J. Eur. Ceram. Soc. 35, 1659–1681 (2015)
J. Zhou, G. Han., Q. Li., Y. Peng., X. Lu., C. Zhang., J. Zhang., Ferroelectric HfZrOx Ge and GeSn PMOSFETs with sub-60mV/decade subthreshold swing, negligible hysteresis, and improved Ids, IEEE International Electron Devices Meeting (IEDM), (IEEE, 2016), pp 12.2.1–12.2.4.
J. Zhou, Z. Zhou, X. Wang, H. Wang, C. Sun, K. Han, Y. Kang, X. Gong, Demonstration of ferroelectricity in Al-doped HfO2 with a low thermal budget of 500 °C. IEEE Electr. Device Lett. 41, 1130–1133 (2020)
Z. Zhou, J. Zhou, X. Wang, H. Wang, C. Sun, K. Han, Y. Kang, Z. Zheng, H. Ni, X. Gong, A metal-insulator-semiconductor non-volatile programmable capacitor based on a HfAlOx ferroelectric film. IEEE Electr. Device Lett. 41, 1837–1840 (2020)
Y. Ma, L. Dong, P. Li, L. Hu, B. Lu, Y. Miao, B. Peng, A. Tian, W. Liu, First-principles-based quantum transport simulations of high-performance and low-power MOSFETs based on monolayer Ga2O3, ACS. Appl. Mater. Interfaces. 14, 48220–48228 (2022)
L. Dong, P. Li, Y. Zhao, Y. Miao, B. Peng, B. Xin, W. Liu, First-principles study on the electronic properties of layered Ga2O3/TeO2 heterolayers for high-performance electronic devices. Appl. Surf. Sci. 602, 154382 (2022)
Z. Hanani, D. Mezzane, M. Amjoud, A.G. Razumnaya, S. Fourcade, Y. Gagou, K. Hoummada, M. El Marssi, M. Gouné, Phase transitions, energy storage performances and electrocaloric effect of the lead-free Ba0.85Ca0.15Zr0.10Ti0.90O3 ceramic relaxor. J. Mater. Sci.-Mater. Electron. 30, 6430–6438 (2019)
X. Ji, C.B. Wang, S. Zhang, R. Tu, Q. Shen, J. Shi, L.M. Zhang, Structural and electrical properties of BCZT ceramics synthesized by sol–gel-hydrothermal process at low temperature. J. Mater. Sci. Mater. Electron. 30, 12197–12203 (2019)
X. Ji, C.B. Wang, S.B. Li, S. Zhang, R. Tu, Q. Shen, J. Shi, L.M. Zhang, Structural and electrical properties of BCZT ceramics synthesized by sol–gel process. J. Mater. Sci. Mater. Electron. 29, 7592–7599 (2018)
J.G. Hao, W.F. Bai, W. Li, J.W. Zhai, Correlation between the microstructure and electrical properties in high-performance (Ba0.85Ca0.15)(Zr0.1Ti0.9)O3 lead-free piezoelectric ceramics. J. Am. Ceram. Soc. 95, 1998–2006 (2012)
M. Dawber, K.M. Rabe, J.F. Scott, Physics of thin-film ferroelectric oxides. Rev. Mod. Phys. 77, 1083–1130 (2005)
N. Setter, D. Damjanovic, L. Eng, G. Fox, S. Gevorgian, S. Hong, A. Kingon, H. Kohlstedt, N.Y. Park, G.B. Stephenson, I. Stolitchnov, A.K. Tagantsev, D.V. Taylor, T. Yamada, S. Streiffer, Ferroelectric thin films: review of materials, properties, and applications. J. Appl. Phys. 100, 051606 (2006)
X.G. Tang, H.L.W. Chan, Effect of grain size on the electrical properties of (ba,ca)(Zr,Ti)O3 relaxor ferroelectric ceramics. J. Appl. Phys. 97, 034109 (2005)
Y.T. Lin, X.R. Miao, N. Qin, H. Zhou, W.L. Deng, D.H. Bao, Effects of Mn doping on structural and dielectric properties of sol–gel-derived (Ba0.835Ca0.165)(Zr0.09Ti0.91)O3 thin films. Thin Solid Films 520, 5146–5150 (2012)
W.S. Choi, J.S. Yi, B.Y. Hong, The effect of cerium doping in barium zirconate titanate thin films deposited by rf magnetron sputtering system. Mat. Sci. Eng. B Solid. 109, 146–151 (2004)
S.R. Reddy, V.V.B. Prasad, S. Bysakh, V. Shanker, N. Hebalkar, S.K. Roy, Superior energy storage performance and fatigue resistance in ferroelectric BCZT thin films grown in an oxygen-rich atmosphere. J. Mater. Chem. C 7, 7073–7082 (2019)
K.I. Mimura, T. Naka, T. Shimura, W. Sakamoto, T. Yogo, Synthesis and dielectric properties of (ba,ca)(Zr,Ti)O3 thin films using metal-organic precursor solutions. Thin Solid Films. 516, 8408–8413 (2008)
E. Khomyakova, S. Wenner, K. Bakken, J. Schultheiss, T. Grande, J. Glaum, M.A. Einarsrud, On the formation mechanism of Ba0.85Ca0.15Zr0.1Ti0.9O3 thin films by aqueous chemical solution deposition. J. Eur. Ceram. Soc. 40, 5376–5383 (2020)
Z. Kong, G. Wang, R. Liang, J. Su, M. Xun, Y. Miao, S. Gu, J. Li, K. Cao, H. Lin, B. Li, Y. Ren, J. Li, J. Xu, H.H. Radamson, Growth and strain modulation of GeSn alloys for photonic and electronic applications. Nanomaterials. 12, 981 (2022)
Y.T. Lin, G.H. Wu, N. Qin, D.H. Bao, Structure, dielectric, ferroelectric, and optical properties of (1 − x)ba(Zr0.2Ti0.8)O3–x(Ba0.7Ca0.3)TiO3 thin films prepared by sol–gel method. Thin Solid Films 520, 2800–2804 (2012)
W.F. Bai, B. Shen, F. Fu, J.W. Zhai, Dielectric, ferroelectric, and piezoelectric properties of textured BZT-BCT lead-free thick film by screen printing. Mater. Lett. 83, 20–22 (2012)
A.J. Haider, T. Alawsi, M.J. Haider, B.A. Taha, H.A. Marhoon, A comprehensive review on pulsed laser deposition technique to effective nanostructure production: trends and challenges. Opt. Quant. Electron. 54, 488 (2022)
H.M. Christen, G. Eres, Recent advances in pulsed-laser deposition of complex oxides. J. Phys. Condens. Mat. 20, 264005 (2008)
S.A. Vanalakar, G.L. Agawane, S.W. Shin, M.P. Suryawanshi, K.V. Gurav, K.S. Jeon, P.S. Patil, C.W. Jeong, J.Y. Kim, J.H. Kim, A review on pulsed laser deposited CZTS thin films for solar cell applications. J. Alloy Compd. 619, 109–121 (2015)
R. Verma, A. Chauhan, K.M. Batoo, R. Kumar, M. Hadi, E.H. Raslan, Structural, morphological, and optical properties of strontium doped lead-free BCZT ceramics. Ceram. Int. 47, 15442–15457 (2021)
X. Ji, C.B. Wang, T. Harumoto, Y.S. Tian, S. Zhang, R. Tu, Q. Shen, J. Shi, Deposition-temperature dependence of structure, ferroelectric property and conduction mechanism of BCZT epitaxial films. Ceram. Int. 47, 3195–3200 (2021)
C.L. Li, Z.H. Chen, Y.L. Zhou, D.F. Cui, Effect of oxygen content on the dielectric and ferroelectric properties of laser-deposited BaTiO3 thin films. J. Phys. Condens. Mat. 13, 5261 (2001)
F. Shi, F. Ji, Effects of oxygen partial pressures on microstructures and compositions of BaO–SrO–ZnO–Nb2O5 thin films by RF-sputtering method. J. Mater. Sci. Mater. Electron. 22, 1483–1489 (2011)
J.L. Wang, Y.S. Lai, S.C. Liou, C.C. Tsai, B.S. Chiou, H.C. Cheng, Ferroelectricity and negative temperature coefficient of resistance in pulsed-laser-deposited (Pb,Sr)TiO3 films. J. Phys. D Appl. Phys. 41, 085304 (2008)
Y. Zhang, H.J. Sun, W. Chen, A brief review of ba(Ti0.8Zr0.2)O3–(Ba0.7Ca0.3)TiO3 based lead-free piezoelectric ceramics: past, present and future perspectives. J. Phys. Chem. Solids 114, 207–219 (2018)
S.R. Reddy, V.V.B. Prasad, S. Bysakh, V. Shanker, J. Joardar, S.K. Roy, Ferroelectric and piezoelectric properties of Ba0.85Ca0.15Ti0.90Zr0.10O3 films in 200 nm thickness range. J. Am. Ceram. Soc. 102, 1277–1286 (2019)
D. Mukherjee, P. Mukherjee, H. Srikanth, S. Witanachchi, Carrier-mediated interaction of magnetic moments in oxygen vacancy-controlled epitaxial Mn-doped ZnO thin films. J. Appl. Phys. 111, 07C318 (2012)
X.J. Wang, Y. Huan, Y.X. Zhu, P. Zhang, W.L. Yang, P. Li, T. Wei, L.T. Li, X.H. Wang, Defect engineering of BCZT-based piezoelectric ceramics with high piezoelectric properties. J. Adv. Ceram. 11, 184–195 (2022)
B.C. Luo, D.Y. Wang, M.M. Duan, S. Li, Growth and characterization of lead-free piezoelectric BaZr0.2Ti0.8O3–Ba0.7Ca0.3TiO3 thin films on Si substrates. Appl. Surf. Sci. 270, 377–381 (2013)
S. Yang, J. Xu, B. Gao, L. Wang, J. Chen, X. Chen, Orientation-dependent phase transition and dielectric properties of Ba0.85Ca0.15Ti0.9Zr0.1O3 thin films. J. Mater. Sci-Mater. Electron. 24, 658–661 (2012)
K. Prabahar, R. Ranjith, A. Srinivas, S.V. Kamat, B. Mallesham, V.L. Niranjani, J.P. Praveen, D. Das, Effect of deposition temperature on the microstructure, ferroelectric and mechanical properties of lead free BCZT ceramic thin films. Ceram. Int. 43, 5356–5361 (2017)
S.R. Reddy, A. Kumar, A.R. James, V.V.B. Prasad, S.K. Roy, Ferroelectric and nano-mechanical properties of the chemical solution deposited lead-free BCZT films. Mat. Sci. Eng. B-Adv. 265, 115037 (2021)
H. Lu, J. Lin, H. Zheng, Superior ferroelectric properties and fatigue resistance in tb modified (BaCa)(ZrTi)O3 film grown on SrTiO3 prepared by pulsed laser deposition. Appl. Surf. Sci. 527, 146892 (2020)
M. Shi, J. Zhong, R. Zuo, Y. Xu, L. Wang, H. Su, C. Gu, Effect of annealing processes on the structural and electrical properties of the lead-free thin films of (Ba0.9Ca0.1)(Ti0.9Zr0.1)O3. J. Alloy Compd. 562, 116–122 (2013)
J.P.B. Silva, J. Wang, G. Koster, G. Rijnders, R.F. Negrea, C. Ghica, K.C. Sekhar, J.A. Moreira, M.J.M. Gomes, Hysteretic characteristics of pulsed laser deposited 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3/ZnO bilayers, ACS Appl. Mater. Interfaces. 10, 15240–15249 (2018)
H. Zhang, E.J. Miller, E.T. Yu, Analysis of leakage current mechanisms in Schottky contacts to GaN and Al0.25Ga0.75 N/GaN grown by molecular-beam epitaxy. J. Appl. Phys. 99, 023703 (2006)
Funding
This work was supported by the Self-innovation Research Funding Project of Hanjiang Laboratory (Grant No. HJL202202A005) and State Key Laboratory of Advanced Technology for Materials Synthesis and Processing (Wuhan University of Technology) (Grant No. 2022-KF-33).
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Ji, X., Peng, Q., Zhang, S. et al. Microstructure, electrical properties and conductivity mechanism of BCZT epitaxial films deposited at different oxygen partial pressure by PLD. J Mater Sci: Mater Electron 34, 1647 (2023). https://doi.org/10.1007/s10854-023-10994-7
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DOI: https://doi.org/10.1007/s10854-023-10994-7