Switching In Ferroelectric Thin Films Research Articles

Reversible Mechanical Switching of Ferroelastic Stripe Domains in Multiferroic Thin Films.

The application potential of ferroelectric thin films largely relies on the controllability of their domain structure. Among the various proposed strategies, mechanical switching is being considered as a potential alternative to replace electrical switching for control of the domain structure of ferroelectric thin films via, e.g., the flexoelectric effect. So far, studies on mechanical switching are confined to out-of-plane polarization switching in ferroelectric thin films, which are in pristine or prepoled single-domain states. In this work, we report reversible in-plane mechanical switching of the monoclinic phase (MC phase) stripe domains in BiFeO3 thin films can be realized by scanning tip force. Via controlling the fast scan direction of the scanning probe microscopy tip and the magnitude of the tip force, the effective trailing field induced by the local tip force can be rotated to consequently switch the net in-plane polarization of the two-variant stripe domain patterns by either 90° or 180°. Moreover, the monoclinic to rhombohedral (MC-R) phase transition occurs during mechanical switching with the distribution of R-phase domains dependent on the switching paths. These results extend our current understanding of the mechanical switching behavior in ferroelectric thin films and should be instructive for their future applications.

Dual-frequency piezoelectric micromachined ultrasound transducer based on polarization switching in ferroelectric thin films

Due to its additional frequency response, dual-frequency ultrasound has advantages over conventional ultrasound, which operates at a specific frequency band. Moreover, a tunable frequency from a single transducer enables sonographers to achieve ultrasound images with a large detection area and high resolution. This facilitates the availability of more advanced techniques that simultaneously require low- and high-frequency ultrasounds, such as harmonic imaging and image-guided therapy. In this study, we present a novel method for dual-frequency ultrasound generation from a ferroelectric piezoelectric micromachined ultrasound transducer (PMUT). Uniformly designed transducer arrays can be used for both deep low-resolution imaging and shallow high-resolution imaging. To switch the ultrasound frequency, the only requirement is to tune a DC bias to control the polarization state of the ferroelectric film. Flextensional vibration of the PMUT membrane strongly depends on the polarization state, producing low- and high-frequency ultrasounds from a single excitation frequency. This strategy for dual-frequency ultrasounds meets the requirement for either multielectrode configurations or heterodesigned elements, which are integrated into an array. Consequently, this technique significantly reduces the design complexity of transducer arrays and their associated driving circuits.

Large ferro–pyro–phototronic effect in 0.5Ba(Zr0.2Ti0.8)O3–0.5(Ba0.7Ca0.3)TiO3 thin films integrated on silicon for photodetection

AbstractCoupling together the ferroelectric, pyroelectric, and photovoltaic characteristics within a single material is a novel way to improve the performance of photodetectors. In this work, we take advantage of the triple multifunctionality shown by 0.5Ba(Zr0.2Ti0.8)O3–0.5(Ba0.7Ca0.3)TiO3 (BCZT), as demonstrated in an Al/Si/SiOx/BCZT/ITO thin‐film device. The Si/SiOx acts as an n‐type layer to form a metal–ferroelectric–insulator–semiconductor heterostructure with the BCZT, and with Al and ITO as electrodes. The photo‐response of the device, with excitation from a violet laser (405 nm wavelength), is carefully investigated, and it is shown that the photodetector performance is invariant with the chopper frequency owing to the pyro‐phototronic effect, which corresponds to the coupling together of the pyroelectric and photovoltaic responses. However, the photodetector performance was significantly better than that of the devices operating based only on the pyro‐phototronic effect by a factor of 4, due to the presence of ferroelectricity in the system. Thus, after a poling voltage of −15 V, for a laser power density of 230 mW/cm2 and at a chopper frequency of 400 Hz, optimized responsivity, detectivity, and sensitivity values of 13.1 mA/W, 1.7 × 1010 Jones, and 26.9, respectively, are achieved. Furthermore, ultrafast rise and fall times of 2.4 and 1.5 µs, respectively, are obtained, which are 35,000 and 36,000 times faster rise and fall responses, respectively, than previous reports of devices with the ferro–pyro–phototronic effect. This is understood based on the much faster ferroelectric switching in ferroelectric thin films owing to the predominant 180° domains in a single direction out of plane.

Why it is Unfortunate that Linear Machine Learning "Works" so well in Electromechanical Switching of Ferroelectric Thin Films.

Machine learning (ML)is relied on for materials spectroscopy. It is challenging to make ML models fail because statistical correlations can mimic the physics without causality. Here, using a benchmark band-excitation piezoresponse force microscopy polarization spectroscopy (BEPS) dataset the pitfalls of the so-called "better", "faster", and "less-biased" ML of electromechanical switching are demonstrated and overcome. Using a toy and real experimental dataset, it is demonstrated how linear nontemporal ML methods result in physically reasonable embedding (eigenvalues) while producing nonsensical eigenvectors and generated spectra, promoting misleading interpretations. A new method of unsupervised multimodal hyperspectral analysis of BEPS is demonstrated using long-short-term memory (LSTM) β-variational autoencoders (β-VAEs) . By including LSTM neurons, the ordinal nature of ferroelectric switching is considered. To improve the interpretability of the latent space, a variational Kullback-Leibler-divergency regularization is imposed . Finally, regularization scheduling of β as a disentanglement metric is leveraged to reduce user bias. Combining these experiment-inspired modifications enables the automated detection of ferroelectric switching mechanisms, including a complex two-step, three-state one. Ultimately, this work provides a robust ML method for the rapid discovery of electromechanical switching mechanisms in ferroelectrics and is applicable to other multimodal hyperspectral materials spectroscopies.

Multilevel polarization switching in ferroelectric thin films

Ferroic order is characterized by hystereses with two remanent states and therefore inherently binary. The increasing interest in materials showing non-discrete responses, however, calls for a paradigm shift towards continuously tunable remanent ferroic states. Device integration for oxide nanoelectronics furthermore requires this tunability at the nanoscale. Here we demonstrate that we can arbitrarily set the remanent ferroelectric polarization at nanometric dimensions. We accomplish this in ultrathin epitaxial PbZr0.52Ti0.48O3 films featuring a dense pattern of decoupled nanometric 180° domains with a broad coercive-field distribution. This multilevel switching is achieved by driving the system towards the instability at the morphotropic phase boundary. The phase competition near this boundary in combination with epitaxial strain increases the responsiveness to external stimuli and unlocks new degrees of freedom to nano-control the polarization. We highlight the technological benefits of non-binary switching by demonstrating a quasi-continuous tunability of the non-linear optical response and of tunnel electroresistance.

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Why it is Unfortunate that "Faster," "Better" and "Less Biased" Linear Machine Learning Models "Work" so well in Electromechanical Switching of Ferroelectric Thin Films

Phase field study on the effect of substrate elasticity on tip-force-induced domain switching in ferroelectric thin films

Tip-force-induced domain switching in ferroelectrics has recently attracted extensive interest as it provides an alternative switching strategy that might ease the problems brought by electrical switching. From the viewpoint of mechanics, substrate elasticity can largely modify the tip-induced deformation of ferroelectric thin films. However, so far, discussions on the influence of substrate elastic properties on such domain switching still remain exclusive. Here, a phase-field model is employed to study the influence of substrate stiffness on the domain switching in BaTiO3 (BTO) thin films, with the strain and stress distributions in BTO thin films and substrates solved by the finite element method. The results demonstrate that the substrate stiffness and loading modes (i.e., pressing and sliding) have a great influence on the symmetry of strain and stress distributions. The switched domain size is highly dependent on the substrate stiffness and loading modes. The switching is more efficient for thin films on a softer substrate. Moreover, the domain could be switched more effectively by the sliding mode under relatively large forces. Our study thus provides a strategy to increase the mechanical switching efficiency of ferroelectric thin films via tuning the substrate elasticity.

Numerical Discretization of Variational Phase Field Model for Phase Transitions in Ferroelectric Thin Films

Phase field methods have been widely used to study phase transitions and polarization switching in ferroelectric thin films. In this paper, we develop an efficient numerical scheme for the variational phase field model based on variational forms of the electrostatic energy and the relaxation dynamics of the polarization vector. The spatial discretization combines the Fourier spectral method with the finite difference method to handle three-dimensional mixed boundary conditions. It allows for an efficient semi-implicit discretization for the time integration of the relaxation dynamics. This method avoids explicitly solving the electrostatic equilibrium equation (a Poisson equation) and eliminates the use of associated Lagrange multipliers. We present several numerical examples including phase transitions and polarization switching processes to demonstrate the effectiveness of the proposed method.

Better, Faster, and Less Biased Machine Learning: Electromechanical Switching in Ferroelectric Thin Films

Machine-learning techniques are more and more often applied to the analysis of complex behaviors in materials research. Frequently used to identify fundamental behaviors within large and multidimensional datasets, these techniques are strictly based on mathematical models. Thus, without inherent physical or chemical meaning or constraints, they are prone to biased interpretation. The interpretability of machine-learning results in materials science, specifically materials' functionalities, can be vastly improved through physical insights and careful data handling. The use of techniques such as dimensional stacking can provide the much needed physical and chemical constraints, while proper understanding of the assumptions imposed by model parameters can help avoid overinterpretation. These concepts are illustrated by application to recently reported ferroelectric switching experiments in PbZr0.2 Ti0.8 O3 thin films. Through systematic analysis and introduction of physical constraints, it is argued that the behaviors present are not necessarily due to exotic mechanisms previously suggested, but rather well described by classical ferroelectric switching superimposed by non-ferroelectric phenomena, such as electrochemical deformation, electrostatic interactions, and/or charge injection.

Tip-force-induced ultrafast polarization switching in ferroelectric thin film: A dynamical phase field simulation

Dynamical phase field simulation is performed to reveal the dynamic characteristics of the tip-force-induced polarization switching in ferroelectric thin films. We demonstrate nontrivial influences of kinetic coefficient μ related to the second-order time derivative term in the dynamic equation of polarization on the mechanical switching behavior. It is found that such a term causes an oscillation feature of the switching process. Two characteristic switching times, i.e., the time when the inversed polarization begins to appear (denoted as τS1) and the time when the fraction of switched (c−) domain is largest during the loading process (denoted as τS2), can be defined to describe the tip-force-induced switching behavior. Both τS1 and τS2 are found to be affected by factors like misfit strain, temperature, and film thickness. Remarkably, the mechanical switching of polarization can be rather fast, with the switching time comparable to that of electrical switching. Due to the nontrivial dynamical effects, other important phenomena are observed: (a) the size and the pattern of switched domain (i.e., cylinder vs ring) in a single-point switching event strongly depend on the loading time, (b) the critical force of mechanical switching may be largely decreased by choosing a proper loading time, and (c) a large and stable domain pattern can still be written by a sweeping tip despite that the switched domain is not stable in the single-point switching event. Our study should provide new insights into the ultrafast phenomena in ferroelectric polarization switching under mechanical stimuli.

Ferroelastic‐Domain‐Assisted Mechanical Switching of Ferroelectric Domains in Pb(Zr,Ti)O3 Thin Films

AbstractA recent breakthrough in mechanical polarization switching provides a valuable handle to achieve nanoscale ferroelectric domain control. This flexoelectric switching is usually observed in ultrathin films (≈10 nm or less in thickness), where a large strain gradient is possible. However, from the point of view of device applications, it will be more attractive to achieve mechanical domain switching in thicker films. Here, it is experimentally demonstrated that by introducing ferroelastic a‐domains in PbZr0.1Ti0.9O3 films the potential barrier against 180° c‐domain switching can be greatly decreased, enabling mechanical ferroelectric domain switching in 50 nm thick films by applying a loading force from an atomic force microscope tip. Moreover, these a‐domains are stable in the c‐domain matrix without further mechanical stressing. This makes it possible to create nanoscale domain wall circuitry. These results shed light on the mechanism of domain switching in ferroelectric thin films and may facilitate the design of mechanically controlled novel ferroelectric devices.

Better, Faster, and Less Biased Machine Learning: Electromechanical Switching in Ferroelectric Thin Films

Better, Faster, and Less Biased Machine Learning: Electromechanical Switching in Ferroelectric Thin Films

Probing the origins of electroresistance switching behavior in ferroelectric thin films

Ferroelectric thin films have been systematically investigated via scanning probe microscopy in recent years. Research indicates that the surface potential is the combined result of injected and polarization charges. The relationships between surface potentials and the two types of charges are usually investigated via scanning Kelvin probe microscopy (SKPM). Typically, SKPM investigations indicate that the surface charge distribution is dominated by injected charges trapped during poling using a conductive AFM tip rather than by polarization charges. The presence of injected charges leads to controversy concerning the origins of resistive switching behavior. In this study, relaxation of injected charges was observed during an optimized thermal treatment. This caused polarization charges to dominate over injected charges. Different electroresistance switching characterizations were observed via conductive atomic force microscopy (C-AFM) of injected and polarization charge-dominated films. Our research extends the methods of distinguishing whether electroresistance switching behavior is driven by charge trapping/detrapping or ferroelectric polarization. This provides an effective approach to classifying the origins of electroresistance switching in ferroelectric thin films by combining piezoelectric force microscopy, SKPM, and C-AFM.

Ferroelastic domain motion by pulsed electric field in (111)/(111¯) rhombohedral epitaxial Pb(Zr0.65Ti0.35)O3 thin films: Fast switching and relaxation

Reversible electric-field induced domain switching in ferroelectric thin films gives rise to a large electromechanical coupling. Despite extensive in situ studies confirming a dominant contribution from domain switching, the speed of the domain wall motion had not been discussed enough. In this study, we performed time-resolved measurement of lattice elongation and non-180\ifmmode^\circ\else\textdegree\fi{} domain switching for an epitaxial rhombohedral $(111)/(11\overline{1})$-oriented ($\mathrm{Pb}(\mathrm{Z}{\mathrm{r}}_{0.65}\mathrm{T}{\mathrm{i}}_{0.35}){\mathrm{O}}_{3}$ film under nanosecond electric field pulses by means of synchrotron x-ray diffraction. Both lattice elongation and non-180\ifmmode^\circ\else\textdegree\fi{} domain switching due to a 200-ns electric pulse were directly observed from the shift of the 222 diffraction position toward a lower angle and the change in the integrated intensity ratio of 222 to $22\overline{2}$ peaks, respectively. The non-180\ifmmode^\circ\else\textdegree\fi{} domain switching also results in an increase of the switchable polarization. Following the removal of the electric field, it is seen that the non-180\ifmmode^\circ\else\textdegree\fi{} domain back switching from 222 to $22\overline{2}$ is sluggish compared to the relaxation of the field-induced lattice strain. This is different from the (100)/(001)-oriented tetragonal epitaxial $\mathrm{Pb}(\mathrm{Zr},\mathrm{Ti}){\mathrm{O}}_{3}$ films, in which no obvious delay was detected. These results show the importance of the direct time-resolved response observation of the crystal structure change with the application of a high-speed electric pulse field to understand the frequency dispersion of the ferroelectric and piezoelectric responses of $\mathrm{Pb}(\mathrm{Zr},\mathrm{Ti}){\mathrm{O}}_{3}$ films.

Effects of dislocations with different locations, orientations and density on domain evolution of ferroelectric thin film: A phase field study

The effects of dislocations on polarization distribution and switching in ferroelectric thin films are discussed based on a modified multi-field coupling theoretical framework that combining the flexoelectric effect and the strain field caused by dislocations. First, the correctness of the model is verified through a study about the effects of different flexocoupling types on domain structures around the dislocations. Then, effects of dislocations with different locations, orientations and density are systematically studied. Dislocations in the film will induce the appearance of a-domain. And the size of the new a-domain depends on the orientations and locations of dislocations. Among [001¯], [101¯] and [100] oriented single dislocations, the size of the new a-domain near the [101¯] oriented dislocation is the largest. It is essential to avoid generating [100] and [101¯] oriented dislocations since the [101¯] oriented dislocations can cause imprint failure and [100] oriented dislocations bring intense pinning effects. As the density of dislocations increases, the pinning effect and imprint behavior becomes stronger. The hysteresis loop of the film with [100] oriented multi-dislocations shows no ferroelectricity once the density reaches a certain limit. These dislocations induced imprint behavior and pinning effect can be eliminated by a larger applied electric field when the dislocation density is low. But when the dislocation density gets higher, the situation is different.

Kinetic control of tunable multi-state switching in ferroelectric thin films

Deterministic creation of multiple ferroelectric states with intermediate values of polarization remains challenging due to the inherent bi-stability of ferroelectric switching. Here we show the ability to select any desired intermediate polarization value via control of the switching pathway in (111)-oriented PbZr0.2Ti0.8O3 films. Such switching phenomena are driven by kinetic control of the volume fraction of two geometrically different domain structures which are generated by two distinct switching pathways: one direct, bipolar-like switching and another multi-step switching process with the formation of a thermodynamically-stable intermediate twinning structure. Such control of switching pathways is enabled by the competition between elastic and electrostatic energies which favors different types of ferroelastic switching that can occur. Overall, our work demonstrates an alternative approach that transcends the inherent bi-stability of ferroelectrics to create non-volatile, deterministic, and repeatedly obtainable multi-state polarization without compromising other important properties, and holds promise for non-volatile multi-state functional applications.