柔性无机铁电薄膜的制备及其应用

蓝顺; 潘豪; 林元华

doi:10.7498/aps.69.20201365

摘要

无机铁电薄膜材料有着优异的电、光特性, 被广泛应用于介电、信息存储、压电、光电等领域. 然而, 基于单晶刚性基底和高温、含氧的合成环境的传统制备工艺, 大大限制了其在柔性电子器件中的应用. 实现无机铁电薄膜材料的柔性化可以将这些材料的性能优势进一步应用到可穿戴电子器件中, 是下一代可穿戴电子器件领域的重要发展方向. 本文综述了无机钙钛矿结构铁电薄膜的柔性化制备工艺, 包括直接在柔性基底上生长和将铁电薄膜从刚性基底上剥离、转印到柔性基底两类. 并介绍了柔性无机铁电薄膜的应用, 对其研究现状及未来发展进行了总结与展望.

关键词:

无机铁电薄膜 /
柔性 /
钙钛矿 /
制备

Abstract

Inorganic ferroelectric films exhibit excellent electric and optic properties, which have been widely used in dielectrics, memory, piezoelectric, photoelectric devices, etc. However, conventional synthesis strategies based on rigid single-crystal substrates severely limit their applications in flexible electronics. Realization of flexible inorganic ferroelectric films can introduce the excellent properties of inorganic ferroelectric materials into flexible devices, which is the developing trend for the next generation of electronic devices. In this review, the strategies to fabricate flexible inorganic perovskite structures’ ferroelectric films are summarized, including 1) direct growth on flexible substrates, 2) transferring ferroelectric film from a rigid substrate to a flexible one. Subsequently, the applications of flexible inorganic ferroelectric films are briefly introduced. Finally, research status, prospects and future development trend of flexible inorganic ferroelectric films are discussed.

Keywords:

作者及机构信息

清华大学材料学院, 新型陶瓷与精细工艺国家重点实验室, 北京　100084

通信作者: 林元华, linyh@tsinghua.edu.cn

基金项目: 国家自然科学基金(批准号: 51729201, 51532003)资助的课题

Authors and contacts

State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

Corresponding author: Lin Yuan-Hua, linyh@tsinghua.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grants Nos. 51729201, 51532003)

文章全文 : translate this paragraph

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施引文献

图 1 PZT/LNO/Ni-Cr柔性薄膜的(a)照片(插图为薄膜结构示意图)和(b)室温10 kHz下的电滞回线^[32]; (c) PLZO柔性薄膜在1000次弯折前后的电滞回线对比(插图为柔性薄膜弯折照片)^[41]; (d) 不同双氧水预处理时长的柔性BTO/Ni膜磁电耦合系数随磁场的变化^[40]

Fig. 1. (a) Photograph of a flexible PZT film (inset: schematic structure illustration) and (b) P-E loop of the PZT film measured at 10 kHz^[32]; (c) P-E loops of a flexible PLZO film before and after 1000 bending cycles (inset: photograph of the bending state of the PLZO film)^[41]; (d) magneto-electric (ME) voltage coefficients of the flexible BTO/Ni assemblies as a function of dc magnetic field^[40]. Plane (a), (b) reprinted with permission from Ref. [32]. Copyright 2016 American Chemical Society. Plane (c) reprinted from Ref. [41], with the permission of AIP Publishing.

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图 2 (a) PhS方法的示意图^[34]; (b) 400 ℃退火的PZT薄膜的P-E回线, 下方插图为非开关部分的贡献, 上方插图为开关部分^[47]; (c) 不同工艺制备的BFO薄膜在140 K, 10 kHz条件下的P-E回线^[34]

Fig. 2. (a) Schematic illustration of the PhS method^[34]; (b) P-E loop of the PZT film annealed at 400 °C, the lower inset of (b) correspond to the non-switching contribution to the polarization, the upper inset correspond to the compensated ferroelectric hysteresis loop^[47]; (c) P-E loops for seeded and seeded + UV-irradiated BFO films measured at 140 K and 10 kHz^[34].

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图 3 PZT(Zr/Ti = 20:80)/SRO/CFO/mica柔性铁电存储器^[65]　(a) 实物图及局部AFM图; (b) 面外θ-2θ扫面结果; (c) 面内Φ扫; (d) RSM图; (e) 断面TEM图像, PZT/SRO和SRO/CFO/mica界面局部放大图以及PZT, SRO和云母的选定区域衍射模式

Fig. 3. PZT(Zr/Ti = 20∶80)/SRO/CFO/mica flexible ferroelectric memory^[65]: (a) Photograph of the flexible ferroelectric device on mica with corresponding AFM image of PZT surface; (b) θ-2θ scan of the heterostructure; (c) Φ scans at PZT {002}, SRO {002}, CFO {004}, and mica {202} diffraction peaks (a.u., arbitrary units); (d) reciprocal space mapping of the heterostructure around the PZT (002) peak (r.l.u., relative lattice units); (e) cross-sectional TEM images of PZT/SRO and SRO/CFO/mica interfaces, and the corresponding selected area electron diffraction patterns.

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图 4 两种不同刻蚀方法示意图　(a)刻蚀基底^[70]; (b) 刻蚀牺牲层^[75]

Fig. 4. Schematic illustration of two etching processes: (a) Etching the substrate^[70]; (b) etching the sacrificial layer^[75]. Plane (a) reprinted with permission from Ref. [70]. Copyright 2010 American Chemical Society.

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图 5 (a) LLO剥离-转印示意图^[87]; (b), (c)使用不同能量激光的LLO工艺转印到PET基底上的PZT薄膜表面的SEM照片, 图(b)和(c)对应的激光能量分别为420和 500 mJ/cm², 标尺为3 μm^[87]

Fig. 5. (a) Schematic diagram of the LLO fabrication process^[87]; (b), (c) SEM images of surfaces of the PZT films transferred to a PET substrate by the LLO process using different energy laser: (b) 420 and (c) 500 mJ/cm²^[87]. Scale bars, 3 μm.

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图 6 石墨烯缓冲层辅助剥离过程示意图^[93]

Fig. 6. Schematic of the process of growing and transferring single-crystalline thin films based on epitaxial graphene buffer layer^[93].

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图 7 BST^[99]柔性薄膜在(a)不同半径弯折时与弯折后的介电频谱(flat-1为初始态, flat-2为r = 5 mm弯折之后; flat-3为r = 2 mm弯折之后)和(b) r = 5 mm时18.6 GHz的介电常数和损耗随弯折次数的变化

Fig. 7. (a) Frequency domain spectroscopy of BST flexible film in the bending states and flat states after bending with different radii (flat 1−3: initial state and flat states after bending at r = 5 mm and 2 mm, respectively); (b) ε_r and tanδ of BST flexible film at 18.6 GHz as a function of bending cycle (r = 5 mm)^[99]. Reprinted with permission from Ref. [99]. Copyright 2019 American Chemical Society.

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图 8 FeRAM^[115]和FeFET^[118]的示意图　(a) P-E回线, 插图为FeRAM结构示意图; (b) FeRAM1疲劳特性; (c) FeFET结构示意图; (d) FeFET的转移特性

Fig. 8. Schematic of FeRAM^[115] and FeFET^[118]: (a) P-E loop and the insert is the schematic illustration of FeRAM; (b) fatigue characterization of FeRAM; (c) the schematic illustration of FeFET; (d) transfer characteristics of the FeFET. Plane (a), (b) reprinted with permission from Ref [115]. Copyright 2019 American Chemical Society. Plane (c), (d) reprinted with permission from Ref [118]. Copyright 2020 American Chemical Society.

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图 9 几种云母基柔性铁电存储器的性能数据对比　(a), (d) PZT (Zr/Ti = 20:80)^[65], (a)不同弯折半径时的P-E回线和(d) 1000次弯折前后拉伸、压缩和平整状态的疲劳性能; (b), (e) BLT^[120], (b) 10000次弯折前后及弯折时的P-E回线和(e)疲劳性能; (c), (f) BFO^[122], (c)不同弯折半径时拉伸、压缩条件下的P-E回线和(f)1000次弯折前后的疲劳性能

Fig. 9. Performance of mica-based flexible ferroelectric memories. (a) P-E loops of PZT (Zr/Ti = 20:80) -based memories with various tensile and compressive radii and (d) fatigue performance at unbent, compressively bent and tensilely bent before and after 1000 cycle conditions^[65]; (b) P-E loops of BLT-based memories at bending state and flat states before and after 10000 cycle conditions and (e) fatigue performance^[120]; (c) P-E loops of BFO-based memories with various compressive and tensile bending radii and (f) fatigue performance an unbent and compressively and tensilely bent for 1000 cycle conditions^[122]. Plane (b), (e) reprinted with permission from Ref. [120]. Copyright 2018 American Chemical Society. Plane (c), (f) reprinted with permission from Ref. [122]. Copyright 2019 American Chemical Society.

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图 10 PZT阵列(a)组成的MOSFET示意图和(b)实际器件照片^[130]

Fig. 10. (a) Schematic illustration of the device that includes a square array of piezoelectric thin-film transducers and (b) photograph of the device laminated on a wrist. Scale bar, 2 cm^[130].

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表 1 最近报道的有代表性的柔性和刚性基底的介电薄膜的储能性能

Table 1. Energy storage properties of recently-reported representative dielectrics on rigid and flexible substrates.

材料	基底	U_e/J·cm^–3	η/%	E_b/MV·m^–1	T_w/℃	疲劳次数	弯折次数
0.25BFO-0.3BTO-0.45STO^[6]	Nb:STO	112	80	490	–100—150	10⁸	—
BCT/BZT multilayer^[108]	Nb:STO	83.9	78.4	800	–100—200	10⁶	—
BZT^[21]	Nb:STO	78.7	80.5	697	–150—200	10⁶	—
PLZT^[109]	LNO/Ni	85	65	450	—	—	—
Mn:NBT-BT-BFO^[110]	Pt/F-mica	81.9	64.4	229	25—200	10⁹	10³ (r = 4 mm)
NKBT/BSMT multilayer^[111]	Pt/F-mica	91	68	303	–50—200	10⁸	10⁴ (r = 4 mm)
BZT^[112]	LSMO/STO/F-mica	65.1	72.9	615	–100—200	10⁶	10³ (r = 4 mm)
PLZT^[113]	LNO/F-mica	40.2	58	200	30—180	10⁷	2 × 10³ (r = 4 mm)

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柔性无机铁电薄膜的制备及其应用