压电力显微镜表征Pb(Mg,Nb)O3-PbTiO3超薄膜弛豫特性

doi:10.15541/jim20240471

无机材料学报 ›› 2025, Vol. 40 ›› Issue (6): 675-682.DOI: 10.15541/jim20240471

压电力显微镜表征Pb(Mg,Nb)O₃-PbTiO₃超薄膜弛豫特性

董晨雨¹(), 郑维杰¹, 马一帆², 郑春艳¹, 温峥¹^,²()

1.物理科学学院, 青岛大学, 青岛 266071
2.电子信息学院, 青岛大学青岛 266071

收稿日期:2024-11-09 修回日期:2025-01-19 出版日期:2025-06-20 网络出版日期:2025-01-24
通讯作者: 温峥, 教授. E-mail: zwen@qdu.edu.cn
作者简介:董晨雨(1999-), 女, 硕士研究生. E-mail: 18244065981@163.com
基金资助:
国家自然科学基金(52372113);山东省泰山学者人才工程(tstp20240511)

Characterizations by Piezoresponse Force Microscopy on Relaxor Properties of Pb(Mg,Nb)O₃-PbTiO₃ Ultra-thin Films

DONG Chenyu¹(), ZHENG Weijie¹, MA Yifan², ZHENG Chunyan¹, WEN Zheng¹^,²()

1. College of Physics, Qingdao University, Qingdao 266071, China
2. College of Electronics and Information, Qingdao University, Qingdao 266071, China

Received:2024-11-09 Revised:2025-01-19 Published:2025-06-20 Online:2025-01-24
Contact: WEN Zheng, professor. E-mail: zwen@qdu.edu.cn
About author:DONG Chenyu (1999-), female, Master candidate. E-mail: 18244065981@163.com
Supported by:
National Natural Science Foundation of China(52372113);Taishan Scholar Program of Shandong Province(tstp20240511)

摘要/Abstract

摘要：

弛豫铁电体因其卓越的介电和压电特性, 在传感器、光电器件、高密度存储器、类脑计算等领域展现出广泛的应用潜力。然而, 纳米尺度超薄膜的弛豫特性研究受到严重漏电流的限制, 基于Sawyer-Tower电路和Positive-Up-Negative-Down(PUND)脉冲波形的测试方法存在显著挑战。本研究提出了一种基于压电力显微镜(Piezoresponse Force Microscopy, PFM)的测试方法, 来研究纳米尺度弛豫薄膜的极化特性。以Pb(Mg,Nb)O₃-PbTiO₃ (PMN-PT)超薄膜为例, 比较了不同厚度的PMN-PT弛豫薄膜与铁电Pb(Zr,Ti)O₃(PZT)薄膜在双频追踪PFM (DART-PFM)测量中On-field和Off-field两种模式下的极化回滞行为。通过调节PFM回线测量中的用于极化读出的交流信号电压振幅, 系统表征了纳米厚度PMN-PT薄膜的弛豫特性。进一步对不同面内应变和厚度的PMN-PT超薄膜进行PFM测试, 发现在较大压缩应变(3.19%)下, 弛豫特性被抑制, 表现出显著的铁电特性, 并观测到铁电-弛豫转变的临界厚度。这些实验结果验证了所提出测试方法的有效性。本研究不仅为超薄膜弛豫特性的探索提供了一种新的表征方法, 也为理解铁电材料的弛豫极化行为奠定了基础, 推动了弛豫铁电材料在低维电子学器件中的应用。

关键词: 弛豫铁电体, 压电力显微镜, PMN-PT, 超薄膜, 极化特性

Abstract:

Relaxor ferroelectrics exhibit extensive applications in sensing technology, optoelectronics, high-density memory storage, and neuromorphic computing, owing to their superior dielectric and piezoelectric characteristics. However, conventional methods, including the Sawyer-Tower circuit and the positive-up-negative-down (PUND) pulse train, prove inadequate for nanoscale ultra-thin films, since the relaxor characteristics may be hindered by substantial leakage currents. In this study, a piezoresponse force microscopy (PFM)-based method for characterizing nanoscale relaxor properties was proposed. Taking ultra-thin Pb(Mg,Nb)O₃-PbTiO₃ (PMN-PT) films as examples, this work compares polarization hysteresis behavior under On-field and Off-field modes of the dual AC resonance tracking (DART) PFM measurements between relaxor PMN-PT and ferroelectric Pb(Zr,Ti)O₃ (PZT) thin films with varying thicknesses. Relaxor characteristics of nanometer-thick PMN-PT films are characterized by modulating amplitude of AC readout to eliminate potential false signals. Furthermore, PFM characterizations of PMN-PT ultra-thin films under different in-plane compressive strains and thicknesses demonstrate that the relaxor characteristics are suppressed and ferroelectric properties are observed at relatively large compressive strains of 3.19%. Additionally, the critical thickness for ferroelectric-relaxor transition is identified. These results verify availability of the proposed PFM-based method for characterizing nanoscale relaxor properties. Therefore, this study not only provides a novel characterization method for exploration of the relaxor in ultra-thin films, but also establishes a foundation for understanding the relaxor polarization behavior in ferroelectric materials, thereby advancing applications of relaxor ferroelectric materials in low-dimensional electronic devices.

Key words: relaxor ferroelectric, piezoresponse force microscope, PMN-PT, ultra-thin film, polarization property

中图分类号:

TQ174

董晨雨, 郑维杰, 马一帆, 郑春艳, 温峥. 压电力显微镜表征Pb(Mg,Nb)O₃-PbTiO₃超薄膜弛豫特性[J]. 无机材料学报, 2025, 40(6): 675-682.

DONG Chenyu, ZHENG Weijie, MA Yifan, ZHENG Chunyan, WEN Zheng. Characterizations by Piezoresponse Force Microscopy on Relaxor Properties of Pb(Mg,Nb)O₃-PbTiO₃ Ultra-thin Films[J]. Journal of Inorganic Materials, 2025, 40(6): 675-682.

图/表 10

图1 (a) PMN-PT/SRO/GSO和PZT/SRO/GSO的XRD图谱(其中PMN-PT和PZT厚度均为100 nm, *代表GSO的(00l)衍射峰, 插图分别为GSO衬底、SRO/GSO、PMN-PT(5 nm)/SRO/GSO、PMN-PT(100 nm)/SRO/GSO薄膜异质结构的AFM表面形貌); (b) 5 nm厚度PMN-PT/SRO/GSO异质结构的截面STEM照片和元素分布图; (c) PMN-PT层的HAADF照片

Fig. 1 (a) XRD patterns of PMN-PT/SRO/GSO and PZT/SRO/GSO heterostructures, where PMN-PT and PZT are both 100 nm thick, in which the * symbols indicate the (00l) Bragg reflections peaks of GSO, with insets showing the AFM surface morphologies of GSO substrate, SRO/GSO, PMN-PT(5 nm)/SRO/GSO, PMN-PT(100 nm)/SRO/GSO thin-film heterostructures; (b) Cross-sectional STEM image and elemental distributions of the 5 nm thick PMN-PT/SRO/GSO heterostructure; (c) HAADF image of the PMN-PT layer

图2 不同厚度PZT (a)和PMN-PT (b)薄膜电容器的电滞回线

Fig. 2 Polarization-electric field hysteresis loops of PZT (a) and PMN-PT (b) thin-film capacitors with different thicknesses

图3 不同厚度PZT、PMN-PT薄膜异质结构的PFM回线表征

Fig. 3 PFM hysteresis characterizations on PZT and PMN-PT thin-film heterostructures with different thicknesses (a) Triangular pulse waveform for PFM test, where the red line represents the DC bias to polarize sample and the blue line represents the AC signal (VAC) used for readout. The polarization is read out in the Off-field mode when the DC bias is zero, and in the On-field mode when the DC bias is non-zero; (b) Sketches of the polarization response of the sample; (c) PFM hysteresis loops with various VAC; (d-g) PFM phases and amplitude hysteresis loops obtained under On-field and Off-field modes with various VAC: 40 nm-thick PZT (d) and PMN-PT (e), 5 nm-thick PZT (f) and PMN-PT (g). Colorful figures are available on website

图4 不同衬底上5 nm厚度PMN-PT薄膜异质结构的PFM回线表征

Fig. 4 PFM hysteresis loops of 5 nm-thick PMN-PT films on various substrates (a) PMN-PT/SRO/GSO; (b) PMN-PT/SRO/DSO; (c) PMN-PT/SRO/STO. Colorful figures are available on website

图5 不同厚度的PMN-PT/SRO/STO薄膜异质结构的PFM回线表征

Fig. 5 PFM hysteresis loops of PMN-PT/SRO/STO heterostructures with different thicknesses

图S1 100 nm厚的PZT和PMN-PT薄膜样品表面形貌和PFM振幅、相位图

Fig. S1 Surface morphologies, PFM amplitudes and phase images of 100 nm-thick PZT and PMN-PT thin films

图S2 100 nm厚的PMN-PT薄膜的PFM回线表征

Fig. S2 S2 PFM hysteresis loops of 100 nm-thick PMN-PT films

图S3 STO晶体的PFM回线

Fig. S3 PFM hysteresis loops of STO crystal

图S4 (a) PMN-PT/SRO/GSO及(b) PMN-PT/SRO/STO PFM读写畴表征

Fig. S4 (a) PMN-PT/SRO/GSO and (b) PMN-PT/SRO/STO PFM read/write domain characterizations

图S5 不同厚度PMN-PT薄膜的PFM回线表征

Fig. S5 PFM hysteresis loops of PMN-PT films with different thicknesses (a) 10 nm; (b) 15 nm; (c) 20 nm

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压电力显微镜表征Pb(Mg,Nb)O₃-PbTiO₃超薄膜弛豫特性

Characterizations by Piezoresponse Force Microscopy on Relaxor Properties of Pb(Mg,Nb)O₃-PbTiO₃ Ultra-thin Films

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