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Recently, flexible electronic devices have attracted extensive attention due to their characteristics of flexibility, miniaturization and portability. Flexible functional oxide thin films with high performance and stability are the basis for high-performance flexible electronic devices. Perovskite lead zirconate titanate Pb(Zr0.53Ti0.47)O3 (PZT) at "morphotropic phase boundary" indicates excellent ferroelectricity and piezoelectricity, and has broad prospects in flexible non-volatile memories, sensors and actuators. Moreover, high-temperature stable flexible memories and sensors have received increasing attention due to the escalating complexity of the external environment. In the present work, Pb(Zr0.53Ti0.47)O3/SrRuO3/BaTiO3 (PZT/SRO/BTO) heterostructures are prepared by pulsed laser deposition on high temperature resistant two-dimensional layered fluorphlogopite mica substrates. Afterward, flexible epitaxial PZT thin films are obtained by mechanical stripping. The ferroelectricity, piezoelectricity and high temperature characteristics of PZT thin films are investigated. The thin films show superior ferroelectricity at room and high temperatures. At room temperature, the thin films exhibit excellent ferroelectricity with a remnant polarization (Pr) of ~
$ {\rm{65}}\;{\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$ . A saturation polarization (Ps) of ~$ {\rm{80}}\;{\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$ and a coercive field (Ec) of ~100 kV/cm are also observed. In addition, after bending the thin films to a 1.5 cm radius 104 times, their ferroelectricity does not show deterioration at room temperature. In order to study the ferroelectricity of PZT thin films at high temperature, P-E loops from 27 ℃ to 275 ℃ are tested. The results show that the films still show excellent ferroelectricity with a Pr of ~$ {\rm{50}}\;{\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$ and a Ps of ~$ {\rm{70}}\;{\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$ at 275 ℃. The present work provides a basis for the application of flexible epitaxial PZT thin film. Especially, the ferroelectricity of flexible PZT thin films at high temperature provides a possibility of obtaining high-temperature flexible electronic devices.-
Keywords:
- Pb(Zr0.53Ti0.47)O3 /
- flexible films /
- high temperature /
- ferroelectric
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图 1 PZT薄膜柔性展示
Figure 1. Flexibility of PZT thin films.
图 2 PZT薄膜XRD图 (a) θ-2θ衍射图; (b) Φ扫描图
Figure 2. (a) θ-2θ scan and (b) Φ-scans of PZT thin films.
图 3 PZT薄膜的(a)表面形貌图, (b)局部极化翻转, (c) 图(b)中白线部分所对应的相位翻转示意图, (d)振幅和相位曲线
Figure 3. (a) Surface morphology, (b) local polarization flipping, (c) intuitive data for white line in (b), (d) representative local PFM amplitude and phase hysteresis loops of PZT thin films.
图 4 (a)不同电场强度下的P-E; (b)样品弯折104次后的P-E; (c)不同温度下的P-E; (d)样品Pr和Ps随温度变化的示意图
Figure 4. (a) P-E loops at various electric fields; (b) P-E loops after bending for 104 times; (c) P-E loops at various temperatures; (d) remnant and saturation polarizations as a function of temperature.
表 1 脉冲激光沉积技术制备PZT/SRO/BTO异质结的实验条件
Table 1. Experimental conditions of PZT/SRO/BTO heterostructure by PLD.
制备工艺 沉积温度/℃ 腔内氧压/Pa 激光能量/mJ 脉冲频率/Hz 沉积时间/min BTO 580 20 100 2 6 SRO 580 20 100 3 20 PZT 600 15 165 4 50 
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[1] Forrest S R 2004 Nature 42 8911
[2] Hou P F, Yang K X, Ni K K, Wang J B, Zhang X L, Liao M, Zheng S Z 2018 J. Mater. Chem. C 6 5193
Google Scholar
[3] Hoffman J, Pan X, Reiner J W, Walker F J, Han J P, Ahn C H, Ma T P 2010 Adv. Mater. 22 295
Google Scholar
[4] Scott J F, Araujo C A P 1989 Science 246 1400
Google Scholar
[5] Jaffe B, Roth R S, Marzullo S 2004 J. Appl. Phys. 2 56
Google Scholar
[6] Kim D J, Maria J P, Kingon A I, Streiffer S K 2003 J. Appl. Phys. 93 5568
Google Scholar
[7] Palneedi H, Yeo H G, Hwang G T, Annapureddy V, Kim J W, Choi J J, Susan T M, Ryu J 2017 APL Mater. 5 0096111
Google Scholar
[8] Bao D H, Zhu X H, Alexe M, Dietrich H 2008 J. Electroceram 21 72
Google Scholar
[9] Wang Y P, Zhou L, Lu X B, Liu Z G 2003 Appl. Surf. Sci. 205 176
Google Scholar
[10] Rho J, Kim S J, Heo W, Lee N E, Lee H S, Ahn J H 2010 Electron Dev. Lett. 31 1017
Google Scholar
[11] Bretos I, Jimenez R, Wu A, Kingon A I, Vilarinho P M, Calzada M L 2014 Adv. Mater. 26 1405
Google Scholar
[12] Aday J, Mendoza M, Lado J L, Joshua O I 2016 Chem. Mater. 28 4042
Google Scholar
[13] Chu Y H 2017 npj Quantum Mater. 2 67
Google Scholar
[14] Jiang J, Bite Y, Huang C W, Do T H, Liu H J, Hsieh Y H, Ma C H, Jang C Y, Lai P W, Wu W W, Chen Y C, Zhou Y C, Chu Y H 2017 Sci. Adv. 3 1700121
Google Scholar
[15] Gao W X, You L, Wang Y J, Yuan G L, Chu Y H, Liu Z G, Liu J M 2017 Adv. Electron 3 1600542
Google Scholar
[16] 胡婷, 阚二军 2018 67 157701
Google Scholar
Hu T, Kan E J 2018 Acta Phys. Sin. 67 157701
Google Scholar
[17] Tommaso G 2018 Nature Mater. 17 846
Google Scholar
[18] Lin S H, Chui Y S, Li Y Y, Lau S P 2017 FlatChem 2 15
Google Scholar
[19] Ohno T, Fukumitsu T, Honda T, Hirai S, Arai T, Sakamoto N, Wakiya N, Suzuki H, Matsuda T 2015 Mater. Lett. 181 74
Google Scholar
[20] Izyumskaya N, Alivov Y I, Cho S J, Morkoc H, Lee H, Kang Y S 2013 Crit. Rev. Solid Mater. Sci. 32 111
Google Scholar
[21] Li C I, Lin J C, Chu M W, Chen H W, Ma C H, Tsai C Y, Huang H W, Lin H J, Liu H L, Chiu P W Chu Y H 2016 Chem. Mater. 28 3914
Google Scholar
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