Piezoresponse Force Microscopy Research Articles

Unraveling the impact of initial choices and in-loop interventions on learning dynamics in autonomous scanning probe microscopy

The current focus in Autonomous Experimentation (AE) is on developing robust workflows to conduct the AE effectively. This entails the need for well-defined approaches to guide the AE process, including strategies for hyperparameter tuning and high-level human interventions within the workflow loop. This paper presents a comprehensive analysis of the influence of initial experimental conditions and in-loop interventions on the learning dynamics of Deep Kernel Learning (DKL) within the realm of AE in scanning probe microscopy. We explore the concept of the “seed effect,” where the initial experiment setup has a substantial impact on the subsequent learning trajectory. Additionally, we introduce an approach of the seed point interventions in AE allowing the operator to influence the exploration process. Using a dataset from Piezoresponse Force Microscopy on PbTiO3 thin films, we illustrate the impact of the “seed effect” and in-loop seed interventions on the effectiveness of DKL in predicting material properties. The study highlights the importance of initial choices and adaptive interventions in optimizing learning rates and enhancing the efficiency of automated material characterization. This work offers valuable insights into designing more robust and effective AE workflows in microscopy with potential applications across various characterization techniques.

Energy storage properties influenced by relaxor ferroelectric properties dependent on the growth direction of epitaxial Bi2SiO5 thin films

Ferroelectric Bi2SiO5 (BSO) thin films were deposited by pulsed laser deposition on Nb-doped (100), (110) and (111) SrTiO3 (Nb:STO) substrates, resulting in (001)-, (113)- and (204)-oriented epitaxial films. Due to the crystallinity of BSO, in which the Bi2O2 layers are formed perpendicular to the c-axis direction, the (001)-oriented epitaxial BSO thin film showed the lowest remanent polarization and the best leakage current characteristics. On the other hand, the (113)- and (204)-oriented films showed an increase in remanent polarization due to the improvement of a-oriented crystallinity. Through experiments using vertical and lateral piezoresponse force microscopy, it has been confirmed that the distribution of in-plane-oriented domains reducing remanent polarization decreases in the order of (001)-, (113)- and (204)-oriented epitaxial BSO thin films. The epitaxial BSO thin films that exhibit ferroelectric hysteresis loops similar to the relaxor ferroelectric thin films tended to have improved energy storage characteristics as a result of improved remanent polarization and saturation polarization. In particular, the (113)-oriented epitaxial BSO thin film showed a high recoverable energy density of about 41.6 J cm−3 and an energy storage efficiency of about 85.6%.

Piezoelectric and Dielectric Electrospun Fluoropolymer Membranes for Oral Mucosa Regeneration: A Comparative Study.

Wound healing of the oral mucosa is an urgent problem in modern dental surgical practice. This research article presents and compares the findings of the investigations of the structural, physicochemical, and biological characteristics of two types of polymeric membranes used for the regeneration of oral mucosa. The membranes were prepared from poly(tetrafluoroethylene) (PTFE) and a copolymer of vinylidene fluoride and tetrafluoroethylene (VDF-TeFE) and analyzed via scanning electron microscopy, atomic force microscopy, X-ray diffraction analysis, and Fourier transform infrared spectroscopy. Investigation results obtained indicate that both types of membranes are composed of thin fibers: (0.57 ± 0.25) μm for PTFE membranes and (0.43 ± 0.14) μm for VDF-TeFE membranes. Moreover, the fibers of VDF-TeFE membranes exhibit distinct piezoelectric properties, which are confirmed by piezoresponse force microscopy and X-ray diffraction. Both types of membranes are hydrophobic: (139.7 ± 2.5)° for PTFE membranes and (133.5 ± 2.0)° for VDF-TeFE membranes. In vitro assays verify that both membrane types did not affect the growth and division of mice fibroblasts of the 3T3-L1 cell line, with a cell viability in the range of 88-101%. Finally, in vivo comparative experiments carried out using Wistar rats demonstrate that the piezoelectric VDF-TeFE membranes have a high ability to regenerate oral mucosa.

Core/Shell-Like Localized Emission at Atomically Thin Semiconductor-Au Interface.

Localized emission in atomically thin semiconductors has sparked significant interest as single-photon sources. Despite comprehensive studies into the correlation between localized strain and exciton emission, the impacts of charge transfer on nanobubble emission remains elusive. Here, we report the observation of core/shell-like localized emission from monolayer WSe2 nanobubbles at room temperature through near-field studies. By altering the electronic junction between monolayer WSe2 and the Au substrate, one can effectively adjust the semiconductor to metal junction from a Schottky to an Ohmic junction. Through concurrent analysis of topography, potential, tip-enhanced photoluminescence, and a piezo response force microscope, we attribute the core/shell-like emissions to strong piezoelectric potential aided by induced polarity at the WSe2-Au Schottky interface which results in spatial confinement of the excitons. Our findings present a new approach for manipulating charge confinement and engineering localized emission within atomically thin semiconductor nanobubbles. These insights hold implications for advancing the nano and quantum photonics with low-dimensional semiconductors.

Single or Vortex Ferroelectric and Ferromagnetic Domain Nanodot Array of Magnetoelectric BiFe0.9Co0.1O3.

Nanodots composed of multiferroic cobalt-substituted BiFeO3, a ferroelectric ferromagnet at room temperature, are fabricated by pulsed laser deposition using anodized porous alumina as masks. The obtained nanodots are approximately 60 nm in diameter, more than 10 nm in thickness, and approximately 70 Gbit/in.2 in density. Piezoresponse and magnetic force microscopies show both ferroelectricity and ferromagnetism with a single-domain nature. It is also found that the dot with 190 nm diameter had multidomain vortex ferroelectric and magnetic structures indicating the strong magnetoelectric coupling. The single-domain cobalt-substituted BiFeO3 nanodots are suitable for verifying magnetization reversal by the electric field, which is the first step in the development of low-power-consumption nonvolatile magnetic memory devices.

An enhanced strain response in micrometer-thick BNT-ST thin films

Lead-free Bi0.5Na0.5TiO3-SrTiO3 (BNT-ST) thin films with various thicknesses were deposited on the Pt(111)/Ti/SiO2/Si(100) substrates employing a sol-gel technique with a two-step annealing process. Despite the variations in thickness, the films exhibited a consistent polycrystalline structure, evidenced by identical diffraction peaks, albeit with differences in intensity. An imprint became evident in micro-thick films, increasing with film thickness. Also, the emergence of self-polarization was observed in thicker films detected by piezoresponse force microscopy. Noteworthy is the pronounced influence of film thickness on strain response, with the 1.38 μm-thick films demonstrating a large strain of 1.18%. The outstanding strain response can be attributed to the notable contribution of electric field-induced phase transition and polarization dynamics. This work provides a promising potential application of micrometer-thick BNT-ST thin films in advanced actuator devices.

Heart rate monitoring system based on piezoelectric poly(vinylidene fluoride-co-trifluoroethylene) composites with barium strontium titanate ceramic particles

A heart rate sensor device has been designed and developed based on a composite material based on poly(vinylidene fluoride – co – trifluoroethylene), P(VDF-TrFE) as polymer matrix and barium strontium titanate (BST) particles as ceramic fillers. The composite films were prepared by solvent casting varying the ceramic particles content between up to 40 wt%, allowing to tailor the dielectric and piezoelectric response. The morphology, polymer phase and thermal properties are independent of the ceramic filler content, whereas the dielectric constant increases significantly with increasing filler content, the largest dielectric constant, ε’ = 38 at 1 kHz, being obtained for the composite with 40 wt% of ceramic particles. Further, the highest piezoelectric response, also dependent on ceramic filler content, is |d33|= 29 pC/N, being obtained for the 10 wt% ceramic particle content film. It is also shown by piezoresponse force microscopy that higher ceramic particles are characterized by more stable ferroelectric domains. The composite has been successfully proved for its potential in heart rate monitoring applications, exhibiting high levels of precision as well as reliability. This work on heart rate sensing presents a material suitable for its incorporation into wearable gadgets, medical devices, and sports equipment, compatible with integration by printing technologies, enabling consumers to access immediate data relevant to their cardiovascular health.

Low temperature sputtering deposition of Al1−xScxN thin films: Physical, chemical, and piezoelectric properties evolution by tuning the nitrogen flux in (Ar + N2) reactive atmosphere

This work investigates the physical properties of Al1−xScxN thin films sputtered at low temperatures by varying the process conditions. Specifically, the films were deposited at room temperature by applying a radio frequency power equal to 150 W to an AlSc alloy (60:40) target, varying the nitrogen flux percentage in the (Ar + N2) sputtering atmosphere (30%, 40%, 50%, and 60%) and keeping constant the working pressure at 5 × 10−3 mbar. The structural and chemical properties of the Al1−xScxN films were studied by x-ray diffraction and Rutherford backscattering spectrometry techniques, respectively. The piezoelectric response was investigated by piezoresponse force microscopy. In addition, the surface potential was evaluated for the first time for Sc-doped AlN thin films by Kelvin probe force microscopy, providing piezoelectric coefficients free from the no-piezoelectric additional effect to the mechanical deformation, i.e., the electrostatic force. By alloying AlN with scandium, the piezoelectric response was strongly enhanced (up to 200% compared to undoped AlN), despite the low deposition temperature and the absence of any other additional energy source supplied to the adatoms during thin film growth, which generally promotes a better structural arrangement of polycrystalline film. This is a strategic result in the field of microelectromechanical systems completely fabricated at low temperatures.

Domain Dynamics and Resistive Switching in Ferroelectric Al1–xScxN Thin Film Capacitors

AbstractIn this paper, using a combination of pulse testing measurements and piezoresponse force microscopy (PFM), an investigation of the polarization reversal behavior and the accompanying resistive switching in the Al0.72Sc0.28N thin film capacitors is reported. The obtained results reveal a transition from the nucleation‐limited switching (NLS) in the low field range toward the more uniform switching described by the Kolmogorov–Avrami–Ishibashi (KAI) model in the high field range. It is found that the Al0.72Sc0.28N capacitors exhibit an unusually steep change in the switching time– it decreases by five orders of magnitude with a moderate increase of the applied field. This feature is caused by a significantly higher activation field value (≈126 MV cm−1) in comparison with the conventional perovskite ferroelectrics. PFM visualization of the field‐induced domain dynamics has allowed the evaluation of the nucleation rate and domain wall velocity. Furthermore, capacitors in the polydomain state generated by partial switching of polarization exhibit a significant (up to two orders of magnitude) increase in the steady‐state conductance. This effect is likely caused by the injection of strongly inclined conducting 180° domain walls. Resistance tunability offers additional functionalities to the Al1‐xScxN devices where conductive domain walls are used as active elements.

The Robust Ferroelectric and Electrical Response in 2D Bi2O2Se Semiconductor

AbstractThe amelioration of atomically thin ferroelectric materials is imperative for next‐generation outperformed two‐dimensional (2D) electronics, which is elusive by their bulk counterparts. These remarkable materials’ ferroelectric and piezoelectric features are the fundamental urges in optoelectronics, electronics, and energy harvesting. In this work, 2D ferroelectric Bi2O2Se flakes have been synthesized using a modified chemical vapor deposition technique. The 6 nm thick Bi2O2Se flake provides a robust ferroelectric switching under an applied voltage of ±10 V by piezoresponse force microscopy, further confirmed by first principles. Leveraging the successful growth, the high‐quality Bi2O2Se flakes permit the fabrication of a field‐effect transistor (FET) with state‐of‐the‐art performance. The FET device rewards a high current on–off ratio of 108 and field effect mobility of almost 131 cm2 V−1 s−1, owing to the small carrier effective mass of 0.2 m0. Combined, the electric field‐induced local polarization of ferroelectric switching and unprecedented device performance of Bi2O2Se semiconductors are certified for their utilization in advanced nanoelectronics and miniaturization of multifunctional devices with multifunctionalities.

Fabrication and characterization of V-doped ZnO films implemented to lead-free piezoelectric micromachined devices

Piezoelectric micromachined ultrasonic transducers (p-MUTs) have been extensively utilized in medical imaging, range-finding, gesture recognition, and so on. However, the piezoelectric layer is dominated by the toxic Pb(Zr, Ti)O3, other materials possess inferior piezoelectric coefficients, and the traditional clamped diaphragm restricts the p-MUT response. In this work, lead-free ZnO films are doped by the vanadium nanostructures and are implemented to beam-island structure membranes, which are aimed to achieve non-toxic and high-performance p-MUTs. Firstly, the doping mechanism of ZnO is analyzed and the p-MUT structure is designed. Secondly, simulation based on the finite element method is conducted to evaluate the dynamic displacement of p-MUTs, after which prototypes are fabricated by the standard micromachined process. The effects of key fabrication parameters including O2 flow rates, sputtering targets, and annealing temperatures on V-doped ZnO films are investigated in detail. By using atomic force microscopy (AFM) and X-ray diffraction (XRD), the surface morphology and crystal structure of the films are analyzed respectively. Moreover, the piezoelectric properties are measured by piezo response force microscopy (PFM). The results indicate a piezoelectric coefficient as high as 194.5 p.m./V, which is superior to most doped ZnO films. Finally, an experimental testing system is established to examine the p-MUT performance. Compared with the clamped diaphragm, the beam-island structure can acquire better electromechanical coupling and achieve range-finding successfully. This work provides a fine application prospect for enhancing the performance of lead-free p-MUTs.

Simultaneously achieved large electrocaloric effect and broad working temperature range in transparent Sm-doped 0.88 Pb(Mg1/3Nb2/3)O3-0.12PbTiO3 ceramics at low electric field

Electrocaloric refrigeration technology has garnered significant attention due to its potential for next-generation solid-state cooling, which is miniaturized and efficient. However, achieving a substantial electrocaloric effect (ECE) and a wide working temperature range at low electric fields remains a challenge. In this study, a synergistic approach combining domain and defect engineering was used in transparent 0.88 Pb(Mg1/3Nb2/3)O3-0.12PbTiO3-xSm(0.88PMN-0.12 PT-xSm) ceramics to improve ECE and temperature stability. Finally, a notable adiabatic temperature change (ΔT) of 2.07 K in the x = 0.01 ceramic, with ΔT exceeding 1.0 K across a broad temperature range from 30 to 180 °C was achieved. Piezoresponse force microscopy (PFM) and X-ray photoelectron spectroscopy revealed the presence of small domains and appropriate oxygen vacancies as contributors to the enhanced ECE and broad operation temperature range. This work introduces a promising candidate material for electrocaloric refrigeration.

Evaluating the optoelectronic properties of individual CsPbBr3 microcrystals by electric AFM techniques

All-inorganic perovskite materials are attracting the attention of researchers owing to the good performance that they exhibit in optoelectronic device applications. In particular, cesium lead halide single crystals are of interest for their electric conductivity. However, the conductive properties of these materials are still far from being fully understood. In this work, we used several scanning probe microscopy techniques to investigate different properties of CsPbBr3 single crystals, namely their topography, electric conductivity, electric surface potential and ferroelectricity. We observed heterogeneity in conductance and work function of the different facets by using conductive atomic force microscopy and Kelvin probe force microscopy measurements. Additionally, piezo-response force microscopy was carried out to gain insight on the origin of the hysteresis in our microcrystals. Our results show the absence of ferroelectric domains and we attribute the I–V hysteresis to ionic migration within the crystal.

Phase transitions in ferroelectric ZrO2 thin films

In this work, the formation of the orthorhombic phase of ZrO2 together with the minor monoclinic phase were elucidated by X-ray diffraction and transmission electron microscopy. Moreover, oxidized W can be responsible for the formation of oxygen vacancies in the ZrO2 through oxygen scavenging. The ferroelectric properties of the W/ZrO2/W film capacitors were investigated through piezoresponse force microscopy (PFM) and polarization-voltage measurements.A second-order phase transition from the polar orthorhombic phase to the non-polar tetragonal phase was observed. Density functional theory calculations confirm our experimental results and propose that oxygen vacancies are responsible for the Curie–Weiss temperature of 130 °C, significantly lower than the theoretical value for the bulk.

Экспериментальные исследования свойств сверхтонких пленок ниобата лития методами зондовой и электронной микроскопии

The article is dedicated to the study of the physical and chemical properties of lithium niobate films made under different temperature conditions. Lithium niobate has already found its application in optics and has enormous potential in various technologies due to the emergence of effects such as piezoelectric effect, nonlinear optical effects, photoelasticity effect, and the Pockels effect (liner electro-optical effect). Lithium niobate can also be used in the oil industry as a catalyst for hydrogenation and dehydrogenation processes, hydrocracking, hydrodesulfurization, and hydroprocessing of oil and petroleum products due to its high surface activity, acidity, and thermal stability, as well as its ability to form stable dispersions in liquid media. The studies were cariied out using scanning electron microscopy technigues, scanning electron microscopy techniques, scanning electron microscopy to study the surface morphology of samples, Kelvin probe microscopy to measure the surface potential of the material, and piezoresponse force microscopy to register the piezoelectric effect of domain structures. As a result of the studies, scans of the surface morphology of samples were obtained, the electrical potential of the surface was measured, and the displacement of samples under the influence of an external elec-tric field with high resolution was also registered. The results of the study can be used to create new materials and devices with high performance and durability, as well as for further development of nanotechnology and nanoelectronics. Further research is planned to investigate other properties of lithium niobate films.

Conducting atomic force microscopy studies on domain wall currents of Bi5 Ti3 FeO15 nanodots fabricated by anodic aluminum oxide nanotemplate and sol-gel process.

We investigated the local current characteristics of Bi5 Ti3 FeO15 (BTFO) nanodots on Nb-doped SrTiO3 substrates affected by their ferroelectric domain structures and domain walls. The BTFO nanodots with a diameter of about 50 nm were fabricated by anodic aluminum oxide nanotemplates and a BTFO sol-gel process. Based on a piezoresponse force microscope, it was confirmed that domain walls were formed in the ferroelectric domain structures of the epitaxial BTFO nanodots. Current changes due to ferroelectric tunneling junctions according to ferroelectric polarizations in epitaxial BTFO nanodots were confirmed by conduction atomic force microscopy. In particular, the domain walls formed in the epitaxial BTFO nanodots formed high currents compared to the currents in ferroelectric tunneling junctions due to polarizations. RESEARCH HIGHLIGHTS: Ferroelectric Bi5 Ti3 FeO15 nanodots with a diameter of 50 nm. Ferroelectric domain structures observed with piezoresponse force microscopy. High domain wall currents observed at domain boundaries observed with conducting atomic force microscopy.

Switchable diode effect in 2D van der Waals ferroelectric CuCrP2S6

Two-dimensional (2D) ferroelectrics has emerged as a promising building block for nonvolatile memory devices. In this work, we demonstrate the out-of-plane ferroelectricity of 2D CuCrP2S6 (CCPS) at the room temperature and the switchable diode effect in 2D CCPS-based ferroelectric nanodevices. The spontaneous out-of-plane ferroelectric polarization switching and hysteresis loops are directly evidenced by the piezoresponse force microscopy. The intrinsic ferroelectricity originates from the non-centrosymmetric structure of 2D CCPS, which is confirmed by optical second-harmonic generation technique. A ferroelectric tunnel junction was built up by using 2D CCPS as a function layer. The observed diode-like forward rectification effect of CCPS diode is opposite to the direction of remnant polarization, which is attributed to the ferroelectric polarization modulation of Schottky barrier. Our work highlights the great potential of 2D CCPS in ultrathin ferroelectric memory device and motivates the development of multifunctional nanodevices.

Mesophase induced by alternating-current poling in relaxor ferroelectric single crystals

Alternating-current poling (AC-Poling) has attracted wide interests in enhancing piezoelectric performance of ferroelectric single crystals. However, the mechanism of phase transformations and domain morphology underlying AC-Poling has not been thoroughly investigated. In this work, we have systematically studied the AC-poling effect on domain structures and piezoelectric properties in the relaxor ferroelectric single crystals of 0.24Pb(In1/2Nb1/2)O3–0.44Pb(Mg1/3Nb2/3)O3–0.32PbTiO3. It is shown that the piezoelectric constant (d33) and permittivity (ε33) are greatly enhanced via [001]-AC-poling compared to DC-poling, related to the presence of modified domain configurations as indicated previously. For [110]-oriented specimens, the piezoelectricity through AC-poling is only half as that for the DC-poled single crystals. We attribute this to the transition from the monoclinic-B phase to an orthorhombic phase under AC-poling, confirmed by synchrotron radiation X-ray diffraction and piezo-response force microscopy. The transition to the orthorhombic phase is likely a consequence of lower Gibbs energy. This study on orientation-dependent characteristics of AC-poling for PIN-PMN-PT single crystals will guide the development of AC-poling technology in applications.

The future of tire energy: a novel one-end cap structure for sustainable energy harvesting

AbstractPiezoelectric energy harvesting is gaining popularity as an eco-friendly solution to harvest energy from tire deformation for tire condition monitoring systems in vehicles. Traditional piezoelectric harvesters, such as cymbal and bridge structures, cannot be used inside tires due to their design limitations. The wider adoption of renewable energy sources into the energy system is increasing rapidly, reflecting a global attraction toward the utilization of sustainable power sources (Aljendy et al. in Int J Power Energy Convers 12(4): 314–337, 2021; Yesner et al. in Evaluation of a novel piezoelectric bridge transducer. In: 2017 Joint IEEE International Symposium on the Applications of Ferroelectric (ISAF)/International Workshop on Acoustic Transduction Materials and Devices (IWATMD)/Piezoresponse Force Microscopy (PFM). IEEE, 2017). The growing interest in capturing energy from tire deformation for Tire Pressure Monitoring Systems (TPMS) aligns with this trend, providing a promising and self-sustaining alternative to traditional battery-powered systems. This study presents a novel one-end cap tire strain piezoelectric energy harvester (TSPEH) that can be used efficiently and reliably inside a tire. The interaction between the tire and energy harvester was analyzed using a decoupled modeling approach, which showed that stress concentration occurred along the edge of the end cap. The TSPEH generated a maximum voltage of 768 V under 2 MPa of load, resulting in an energy output of 32.645 J/rev under 1 MPa. The computational findings of this study were consistent with previous experimental investigations, confirming the reliability of the numerical simulations. The results suggest that the one-end cap structure can be an effective energy harvester inside vehicle tires, providing a valuable solution for utilizing one-end cap structures in high-deformation environments such as vehicle tires.

Kinetics of N- to M-Polar Switching in Ferroelectric Al1-x Scx N Capacitors.

Ferroelectric wurtzite-type aluminum scandium nitride (Al1-x Scx N) presents unique properties that can enhance the performance of non-volatile memory technologies. The realization of the full potential of Al1-x Scx N requires a comprehensive understanding of the mechanism of polarization reversal and domain structure dynamics involved in the ferroelectric switching process. In this work, transient current integration measurements performed by a pulse switching method are combined with domain imaging by piezoresponse force microscopy (PFM) to investigate the kinetics of domain nucleation and wall motion during polarization reversal in Al0.85 Sc0.15 N capacitors. In the studied electric field range (from 4.4 to 5.6MVcm-1 ), ferroelectric switching proceeds via domain nucleation and wall movement. The currently available phenomenological models are shown to not fully capture all the details of the complex dynamics of polarization reversal in Al0.85 Sc0.15 N. PFM reveals a non-linear increase of both domain nucleation rate and lateral wall velocity during the switching process, as well as the dependency of the domain pattern on the polarization reversal direction. A continuously faster N- to M-polar switching upon cycling is reported and ascribed to an increasing number of M-polar nucleation sites and density of domain walls.