柔性Pb(Zr0.53Ti0.47)O3薄膜的高温铁电特性

李敏; 时鑫娜; 张泽霖; 吉彦达; 樊济宇; 杨浩

doi:10.7498/aps.68.20181967

摘要

随着柔性电子产品的迅速发展, 具有优异铁电和压电性的Pb(Zr_0.53Ti_0.47)O₃ (PZT)薄膜在柔性的非易失性存储器、传感器和制动器等器件中有广泛的应用前景. 同时, 由于外部环境越来越复杂, 具有高温稳定特性的材料和器件受到越来越多的关注. 本文在耐高温的二维层状氟晶云母衬底上, 用脉冲激光沉积技术制备出外延的PZT薄膜, 并通过机械剥离的方法, 得到柔性的外延PZT薄膜. 研究了Pt/PZT/SRO异质结的铁电和压电性及其高温特性, 发现样品表现出优越的铁电性, 剩余极化强度(P_r)高达65 ${\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$, 在弯曲10⁴次后其铁电性基本保持不变, 且样品在275 ℃高温时仍然保持良好的铁电性. 本文为柔性PZT薄膜在航空航天器件中的应用提供了实验基础.

关键词:

Abstract

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(Zr_0.53Ti_0.47)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(Zr_0.53Ti_0.47)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 (P_r) of ~$ {\rm{65}}\;{\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$. A saturation polarization (P_s) of ~$ {\rm{80}}\;{\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$ and a coercive field (E_c) 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 P_r of ~$ {\rm{50}}\;{\text{μ}} {\rm{C/c}}{{\rm{m}}^{\rm{2}}}$ and a P_s 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:

作者及机构信息

南京航空航天大学理学院, 南京　210016

通信作者: 杨浩, yanghao@nuaa.edu.cn

基金项目: 国家自然科学基金(批准号: 11774172, U1632122, 51602152)、中央高校基本科研业务费专项基金(批准号: NE2016102, NP2017103)和南京航空航天大学研究生创新基地(实验室)开放基金(批准号: kfjj20170801)资助的课题.

Authors and contacts

College of Science, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China

Corresponding author: Yang Hao, yanghao@nuaa.edu.cn

Funds: Project supported by the National Nature Science Foundation of China (Grant Nos. 11774172, U1632122, 51602152), the Fundamental Research Funds for the Central Universitiesof Ministry of Education of China (Grant Nos. NE2016102, NP2017103), and the Foundation of Graduate Innovation Center in Nanjing University of Aeronautics and Astronautics, China (Grant No. kfjj20170801).

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参考文献

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施引文献

图 1 PZT薄膜柔性展示

Fig. 1. Flexibility of PZT thin films.

下载: 全尺寸图片幻灯片

图 2 PZT薄膜XRD图　(a) θ-2θ衍射图; (b) Φ扫描图

Fig. 2. (a) θ-2θ scan and (b) Φ-scans of PZT thin films.

下载: 全尺寸图片幻灯片

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

Fig. 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.

下载: 全尺寸图片幻灯片

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P_r和P_s随温度变化的示意图

Fig. 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.

下载: 全尺寸图片幻灯片

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

下载: 导出CSV

[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 物理学报 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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柔性Pb(Zr_0.53Ti_0.47)O₃薄膜的高温铁电特性