锆酸铅基反铁电薄膜研究现状与展望

张天富; 司洋洋; 黎意杰; 陈祖煌

doi:10.7498/aps.72.20230389

摘要

距离发现反铁电已有70多年的历史, 其独特的电场诱导相变行为使其在储能、换能器、驱动器、电卡制冷、负电容晶体管、热管理等领域显示出了巨大的应用价值. 随着薄膜生长技术的发展及器件小型化、集成化趋势的需求, 反铁电薄膜受到越来越多的关注. 大量研究表明, 反铁电从块体到薄膜显现出与块体不同的新奇物性, 同时也面临更多挑战, 如尺寸效应使得其反铁电特性在临界厚度下减弱甚至消失等. 在此基础上, 回顾了锆酸铅基反铁电研究的发展历史, 从反铁电的起源、结构、相变到应用等方面进行了讨论. 希望能够吸引更多的研究者关注反铁电薄膜的发展, 探索未知的奥秘, 共同开发更多的新材料和新应用.

关键词:

反铁电 /
锆酸铅 /
结构 /
应用

Abstract

It has been more than 70 years since the first anti-ferroelectric was discovered. Its unique electric-field-induced phase transition behavior shows great potential applications in the fields of energy storage, electrocaloric, negative capacitance, thermal switching, etc. With the development of advanced synthesis technology and the trend of miniaturization and integration of devices, high-quality functional oxide films have received more and more attention. A large number of studies have shown that anti-ferroelectric thin film exhibits more novel properties than bulk, but it also faces more challenges, such as the disappearance of antiferroelectricity under a critical thickness induced by size effect. In this paper, we review the development history of lead zirconate-based anti-ferroelectric thin films, and discuss their structures, phase transitions and applications. We hope that this paper can attract more researchers to pay attention to the development of anti-ferroelectric thin films, so as to develop more new materials and explore new applications.

Keywords:

作者及机构信息

哈尔滨工业大学(深圳)材料科学与工程学院, 深圳　518055

通信作者: 陈祖煌, zuhuang@hit.edu.cn

基金项目: 广东省基础与应用基础研究基金(批准号: 2020B1515020029)、深圳市科技创新项目(批准号: JCYJ20200109112829287)、中国博士后科学基金(批准号: 2022T150158)、广东省重大人才工程引进类(批准号: 2019QN01C202)和深圳市科技计划(批准号: KQTD20200820113045083)资助的课题.

Authors and contacts

School of Materials Science and Engineering, Harbin Institute of Technology, Shenzhen 518055, China

Corresponding author: Chen Zu-Huang, zuhuang@hit.edu.cn

Funds: Project supported by the Guangdong Basic and Applied Basic Research Foundation, China (Grant No. 2020B1515020029), the Shenzhen Science and Technology Innovation Project, China (Grant No. JCYJ20200109112829287), the China Postdoctoral Science Foundation (Grant No. 2022T150158), the Guangdong Major Talent Introduction Project, China (Grant No. 2019QN01C202), and the Shenzhen Science and Technology Program, China (Grant No. KQTD20200820113045083)

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施引文献

图 1 PbZrO₃基反铁电体的重要进展

Fig. 1. Important developments of PbZrO₃ based antiferroelectric.

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图 2 Pb(Zr, Ti)O₃^[46] (a)和(Pb, La)(Zr, Ti)O₃^[47] (b)的二元相图; Pb_0.99Nb_0.02(Zr, Sn, Ti)_0.98O₃^[48] (c)和(Pb_0.97La_0.02)(Zr, Sn, Ti)O₃ ^[48] (d)的三元相图

Fig. 2. Binary phase diagram for Pb(Zr, Ti)O₃^[46] (a) and (Pb, La)(Zr, Ti)O₃^[47] (b); ternary phase diagram for Pb_0.99Nb_0.02(Zr, Sn, Ti)_0.98O₃ ^[48] (c) and Pb_0.97La_0.02(Zr, Sn, Ti)O₃^[48] (d).

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图 3 (a) 改变电子束辐照时间同一区域PZO薄膜的相变行为^[54]; (b) 从(001)和(042)取向PZO薄膜中铅离子位移提取的极化构型^[11]; (c) 不同生长氧压 (120, 80和45 mTorr, 1 Torr = 133.32 Pa) PZO薄膜的极化行为^[55]

Fig. 3. (a) Phase-boundary-driven phase transition in PZO films under the irradiation of an electron beam^[54]; (b) polarization configurations extracted from Pb ions displacements in (001) and (042) oriented PZO films^[11]; (c) polarization-electric field loops of PZO grown at various oxygen pressures (120, 80 and 45 mTorr, 1 Torr = 133.32 Pa)^[55].

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图 4 (a) PZO块体的介电温谱图^[8]; (b) PZO基反铁电薄膜的C-V特性曲线^[59]; (c) PZO薄膜的P-E和I-E回线^[52]; (d) PZO薄膜在直流电场E_DC和交流电场E_AC作用下的电致应变和压电系数^[11]

Fig. 4. (a) Temperature dependent dielectric spectrum of PZO bulk materials, reproduced from^[8]; (b) C-V characteristics of PZO based AFE thin films^[59]; (c) P-E and I-E loops of PZO thin films^[52]; (d) electromechanical response as strain and effective longitudinal piezoelectric coefficient as a function of E_AC and E_DC, respectively^[11].

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图 5 (a) Kittel提出的双子晶格模型; (b) 不同组合多态软模的能量^[62]; (c) PZO中可能存在的调制结构及其能量^[31]; (d) AFE/FE能量与PZO薄膜厚度的关系^[71]

Fig. 5. (a) Antiferroelectric structure model proposed by Kittel; (b) energy difference for different combination of multisoft mode^[62]; (c) proposed modulation structure in PZO and the corresponding energy^[31]; (d) dependence of the AFE/FE energy on thickness of PZO thin film^[71].

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图 6 (a) 不同储能装置的对比示意图; (b) 储能电容器的部分应用场景; (c) 5种常见的电介质材料及其储能示意图

Fig. 6. (a) Ragone plot of different energy storage devices; (b) applications for energy storage capacitors; (c) five distinctive dielectric materials and their energy storage performance.

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图 7 (a) 异价元素Ta掺杂AgNbO₃前后Ag和Nb原子±$[1\overline 1 0]$方向位移波动^[84]; (b) 异价元素Ta掺杂AgNbO₃前后击穿电场、极化强度、储能密度、储能效率的对比^[84]; (c) 离子轰击PZO反铁电薄膜前后的击穿电场和储能对比^[85]

Fig. 7. (a) Ag and Nb atoms displacement fluctuations along ±$[1\overline 1 0]$ of pure AgNbO₃ and Ta doped AgNbO₃^[84]; (b) comparison of breakdown field, polarization, efficiency and energy storage density of pure AgNbO₃ and Ta doped AgNbO₃^[84]; (c) comparison of energy storage performance of PZO thin film before and after ion bombardment^[85].

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图 8 (a) 电卡效应制冷的卡诺循环; (b) PbZr_0.95Ti_0.05O₃薄膜中的电卡温度变化∆T^[111]; (c) 电场响应的PbZrO₃相图及∆T-∆S示意图^[119]

Fig. 8. (a) Carnot cycle of electrocaloric effect refrigeration; (b) temperature change ∆T in PbZr_0.95Ti_0.05O₃ thin film^[111]; (c) tentative phase diagram for PbZrO₃ as a function of electric field and schematic ∆T-∆S diagram^[119].

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图 9 (a) 电致应变的4个主要组成部分; (b) Pb_0.98La_0.02(Zr_0.66Ti_0.10Sn_0.24)_0.995O₃反铁电陶瓷相变过程中应变与电场的关系^[123]; PLZST单晶(c)极化和(d)应变在选定温度下对电场的响应^[45]

Fig. 9. (a) The four main components of electro-strain; (b) strain as a function of electric field during phase transition in Pb_0.98La_0.02(Zr_0.66Ti_0.10Sn_0.24)_0.995O₃ ceramic, reproduced from^[123]; (c) polarization and (d) strain loops of the PLZST single crystals at selected temperatures measured at 1 Hz^[45].

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图 10 (a) 反铁电双电滞回线, 其中BC和B'C'呈现出负电容行为^[132]; (b) 反铁电随机存取存储器的4个可选读出状态^[135]; (c) 反铁电隧道结的示意图^[13]; (d) PZO薄膜实时高低热导率转变^[4]; (e) PZO电容器的稳态光伏响应, 显示超过100 V的开路光电压^[12]

Fig. 10. (a) P-E loop of an antiferroelectric material, segments BC and B'C' represent the unstable negative capacitance (C < 0) regions^[132]; (b) four pseudo-remanent memory states marked on the loop in AFRAM^[135]; (c) schematic representations of expected behaviors of antiferroelectric tunnel junctions^[13]; (d) real-time switching of epitaxial PZO to low and high thermal conductivity^[4]; (e) steady-state photovoltaic response of PZO capacitor, showing an open-circuit photovoltage in excess of 100 V^[12].

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map

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