Signal formation mechanism of Piezoresponse Force Microscopy of piezoelectric surface layers and thin films on stiff and elastically matched substrates is analyzed and thickness dependence of effective piezoelectric response, object transfer function components and Rayleigh two-point resolution are derived. Obtained exact series and simple Pade approximations can be applied for the effective piezoresponse analytical calculations in the case of films capped on different substrates. The effective piezoresponse is thickness dependent for piezoelectric films on substrates with low dielectric permittivity (extrinsic size effect), whereas the thickness dependence is essentially suppressed for giant permittivity or metallic substrates. Thus implications of analysis for ferroelectric data storage and device applications are discussed.
Piezoresponse force microscopy (PFM) is a powerful tool for probing nanometer-scale ferroelectric and piezoelectric properties. Hysteretic switching of the phase and amplitude of the PFM response are believed to be the hallmark of ferroelectric and piezoelectric behavior respectively. However, the application of PFM is limited by the fact that similar hysteretic effects may also arise from mechanisms not related to ferroelectricity or piezoelectricity. In this paper we report our studies on regular glass slides that show ferroelectric-like signal without being ferroelectric and frequently used…
Piezoresponse force microscopy (PFM) has been used extensively for exploring nanoscale ferro/piezoelectric phenomena over the past two decades. The imaging mechanism of PFM is based on the detection of the electromechanical (EM) response induced by the inverse piezoelectric effect through the cantilever dynamics of an atomic force microscopy. However, several non-piezoelectric effects can induce additional contributions to the EM response, which often lead to a misinterpretation of the measured PFM response. This review aims to summarize the non-piezoelectric origins of the EM response that im…
Mitigating parasitic contributions in measured piezoresponse for accurate determination of piezoelectric coefficients in Sc-alloyed-AlN thin films using piezo-response force microscopy
We report the development and experimental implementation of the automated experiment workflows for the identification of the best predictive channel for a phenomenon of interest in spectroscopic measurements. The approach is based on the combination of ensembled deep kernel learning for probabilistic predictions and a basic reinforcement learning policy for channel selection. It allows the identification of which of the available observational channels, sampled sequentially, are most predictive of selected behaviors, and hence have the strongest correlations. We implement this approach for mu…
Correlated domain and crystallographic orientation mapping in uniaxial ferroelectric polycrystals by interferometric vector piezoresponse force microscopy
NTNU Norwegian University of Science and Technology（挪威科技大学）；Asylum Research an Oxford Instruments Company（阿苏姆研究（牛津仪器旗下公司））；University of Duisburg-Essen（杜伊斯堡-埃森大学）；Research Center Future Energy Materials and Systems, Research Alliance Ruhr（鲁尔研究联盟未来能源材料与系统研究中心）
Piezoresponse Force Microscopy (PFM), as a powerful nanoscale characterization technique, has been extensively utilized to elucidate diverse underlying physics of ferroelectricity. However, the intensive study of conventional PFM has revealed a growing number of concerns and limitations which are largely challenging its validity and application. Herein, we developed a new advanced PFM technique, named Heterodyne Megasonic Piezoresponse Force Microscopy (HM-PFM), which uniquely uses 106 to 108 Hz high-frequency excitation and heterodyne method to measure the piezoelectric strain at nanoscale. W…
The interplay between electrochemical surface charges and bulk ferroelectricity in thin films gives rise to a continuum of coupled ferro-ionic states. These states are exquisitely sensitive to chemical and electric conditions at the surfaces, applied voltage, and oxygen pressure. Using the analytical approach combining the Ginzburg-Landau-Devonshire description of the ferroelectricity with Langmuir adsorption isotherm for the ions at the film surface, we have studied the temperature-, time- and field- dependent polarization changes and electromechanical response of the ferro-ionic states. The …
Piezoresponse force microscopy (PFM) has been extensively utilized as a versatile and an indispensable tool to understand and analyze nanoscale ferro- /piezoelectric properties by detecting the local electromechanical response on a sample surface. However, it has been discovered that the electromechanical response not only originates from piezoelectricity but also from other factors such as the electrostatic effect. In this study, we explore the dependence of off-field PFM hysteresis loops on the surface-potential-induced electrostatic effect in a prototypical ferroelectric thin film by applyi…
The presence of electrostatic forces and associated artifacts complicates the interpretation of piezoresponse force microscopy (PFM) and electrochemical strain microscopy (ESM). Eliminating these artifacts provides an opportunity for precisely mapping domain wall structures and dynamics, accurately quantifying local piezoelectric coupling coefficients, and reliably investigating hysteretic processes at the single nanometer scale to determine properties and mechanisms which underly important applications including computing, batteries and biology. Here we exploit the existence of an electrostat…
Combination of local heating and biasing at the tip-surface junction in temperature-assisted piezoresponse force microscopy (tPFM) opens the pathway for probing local temperature induced phase transitions in ferroics, exploring the temperature dependence of polarization dynamics in ferroelectrics, and potentially discovering coupled phenomena driven by strong temperature- and electric field gradients. Here, we analyze the signal formation mechanism in tPFM and explore the interplay between thermal- and bias-induced switching in model ferroelectric materials. We further explore the contribution…
Domain Nucleation and Hysteresis Loop Shape in Piezoresponse Force Spectroscopy
压电响应力显微镜（Piezoresponse Force Microscopy）中的机电磁滞回线测量已经成为探测纳米尺度上的铁电开关行为的强大技术。PFS数据的解释需要建立域参数和PFM信号之间的关系。在这里，我们分析了开关过程中使用修改后的点电荷模型的电场的提示。选择电荷值和位置，使得其电场等势面以确定的曲率半径再现尖端。利用线性弹性理论，推导了半椭球畴大小与PFM信号大小的关系。确定了畴形核对压电响应迟滞回线的作用。
The frequency-dependent amplitude and phase in piezoresponse force microscopy (PFM) measurements are shown to be a consequence of the Euler-Bernoulli (EB) dynamics of atomic force microscope (AFM) cantilever beams used to make the measurements. Changes in the cantilever mode shape as a function of changes in the boundary conditions determine the sensitivity of cantilevers to forces between the tip and the sample. Conventional PFM and AFM measurements are made with the motion of the cantilever measured at one optical beam detector (OBD) spot location. A single OBD spot location provides a limit…
The local hysteresis loop obtained by switching spectroscopy piezoresponse force microscopy (SS-PFM) is usually regarded as a typical signature of ferroelectric switching. However, such hysteresis loops were also observed in a broad variety of non-ferroelectric materials in the past several years, which casts doubts on the viewpoint that the local hysteresis loops in SS-PFM originate from ferroelectricity. Therefore, it is crucial to explore the mechanism of local hysteresis loops obtained in SS-PFM testing. Here we proposed that non-ferroelectric materials can also exhibit amplitude butterfly…
Hafnium oxide (HfO2)-based ferroelectrics offer remarkable promise for memory and logic devices in view of their compatibility with traditional silicon CMOS technology, high switchable polarization, good endurance and thickness scalability. These factors have led to steep rise in research on this class of materials over the past number of years. At the same time, only a few reports on the direct sensing of nanoscale ferroelectric properties exist, with many questions remaining regarding the emergence of ferroelectricity in these materials. While piezoresponse force microscopy (PFM) is ideally …
Domains walls and topological defects in ferroelectric materials have emerged as a powerful new paradigm for functional electronic devices including memory and logic. Similarly, wall interactions and dynamics underpin a broad range of mesoscale phenomena ranging from giant electromechanical responses to memory effects. Exploring the functionalities of individual domain walls, their interactions, and controlled modifications of the domain structures is crucial for applications and fundamental physical studies. However, the dynamic nature of these features severely limits studies of their local …
Detection of dynamic surface displacements associated with local changes in material strain provides access to a number of phenomena and material properties. Contact resonance-enhanced methods of Atomic Force Microscopy (AFM) have been shown capable of detecting ~1-3 pm-level surface displacements, an approach used in techniques such as piezoresponse force microscopy, atomic force acoustic microscopy, and ultrasonic force microscopy. Here, based on an analytical model of AFM cantilever vibrations, we demonstrate a guideline to quantify surface displacements with a high accuracy by taking into …
A nanometric needle sensor mounted in an Atomic Force Microscopy allows systematic picometer-range distance measurements. This force sensing device is used in Piezoresponse Force Microscopy (PFM) as a distance sensor, by employing the cantilever spring constant as the conversion factor opening a pathway to explore the piezoelectric effect at the nanoscale. The force-distance equivalence is achieved if the force sensor does not disturb the system to study, solely. In this manuscript we report a systematic study in which different Lead Zirconate Titanate (PZT) materials, having different d33 val…
Piezoresponse Force Microscopy is a powerful but delicate nanoscale technique that measures the mechanical response resulting from the application of a highly localized electric field. Though mechanical response is normally due to piezoelectricity, other physical phenomena, especially electrostatic interaction, can contribute to the signal read. We address this problematic through the use of longer ultra-stiff probes providing state of the art sensitivity, with the lowest electrostatic interaction and avoiding working in high frequency regime. In order to find this solution we develop a theore…
Domain Switching on the Pareto Front: Multi-Objective Deep Kernel Learning in Automated Piezoresponse Force Microscopy
University of Tennessee（田纳西大学）；Institute of Science Tokyo（东京科学大学）；University of California, Berkeley（加州大学伯克利分校）；Rice University（莱斯大学）；Pacific Northwest National Laboratory（太平洋西北国家实验室）
This paper presents multiple-modes Scanning Probe Microscopy (SPM) studies on characterize resistance switching (RS), polarization rotation (PO) and surface potential changes in copper doped ZnO (ZnO:Cu) thin films. The bipolar RS behavior is confirmed by conductive Atomic Force Microscopy (c-AFM). The PO with almost 180° phase angle is confirmed by using the vertical and lateral Piezoresponse Force Microscopy (PFM). In addition, it elucidates that obvious polarization rotation behavior can be observed in the sample with increasing Cu concentration. Furthermore, correlation of the RS behavior …
Piezoresponse force-microscopy (PFM) has become the standard tool to investigate ferroelectrics on the micro- and nanoscale. However, reliability of PFM signals is often problematic and their quantification is challenging and thus not widely applied. Here, we present a study of the reproducibility of PFM signals and of the so-called PFM background signal which has been reported in literature. We find that PFM signals are generally reproducible to certain extents. The PFM signal difference between 180° domains on periodically-poled lithium niobate (PPLN) is taken as the reference signal in a la…
Ferroelectrics are technologically important, with wide application in micromechanical systems, nonlinear optics, and information storage. Recent discoveries of exotic polarisation textures in these materials, which can strongly influence their properties, have brought to the forefront questions about the nature of their domain walls -- long believed to be primarily Ising, with locally null polarisation. Here, combining three complementary techniques -- second harmonic generation microscopy, piezoresponse force microscopy, and transmission electron microscopy - to cover all the relevant length…
Lateral piezoelectric response across ferroelectric domain walls in thin films
在纯c轴取向的PbZr $_{0.2}$ Ti $_{0.8}$ O $_3$铁电薄膜中，在180°畴壁位置观察到横向压电响应力显微镜信号，在此位置，面外取向的极化被反转。使用电力显微镜测量，我们排除静电效应作为这个信号的起源。此外，我们的机械模拟的尖端/悬臂梁系统表明，小倾斜的表面在域壁下面的尖端不能令人满意地解释所观察到的信号。因此，我们属性在畴壁的横向压电响应，其横向运动（剪切）下施加的电场。从简单的弹性考虑和单位晶胞的体积守恒，我们将预期在其他铁电材料中更普遍地类似的横向信号，并且对于所有类型的畴壁，其中极化的面外分量通过畴壁反转。我们表明，在BiFeO $_3$薄膜，与180，109和71°畴壁，这确实是这种情况。
