Ferroelectric domain-wall logic units

The electronic conductivities of ferroelectric domain walls have been extensively explored over the past decade for potential nanoelectronic applications. However, the realization of logic devices based on ferroelectric domain walls requires reliable and flexible control of the domain-wall configuration and conduction path. Here, we demonstrate electric-field-controlled stable and repeatable on-and-off switching of conductive domain walls within topologically confined vertex domains naturally formed in self-assembled ferroelectric nano-islands. Using a combination of piezoresponse force microscopy, conductive atomic force microscopy, and phase-field simulations, we show that on-off switching is accomplished through reversible transformations between charged and neutral domain walls via electric-field-controlled domain-wall reconfiguration. By analogy to logic processing, we propose programmable logic gates (such as NOT, OR, AND and their derivatives) and logic circuits (such as fan-out) based on reconfigurable conductive domain walls. Our work provides a potentially viable platform for programmable all-electric logic based on a ferroelectric domain-wall network with low energy consumption.

Piezoelectricity in hafnia

Because of its compatibility with semiconductor-based technologies, hafnia (HfO2) is today’s most promising ferroelectric material for applications in electronics. Yet, knowledge on the ferroic and electromechanical response properties of this all-important compound is still lacking. Interestingly, HfO2 has recently been predicted to display a negative longitudinal piezoelectric effect, which sets it apart from classic ferroelectrics (e.g., perovskite oxides like PbTiO3) and is reminiscent of the behavior of some organic compounds. The present work corroborates this behavior, by first-principles calculations and an experimental investigation of HfO2 thin films using piezoresponse force microscopy. Further, the simulations show how the chemical coordination of the active oxygen atoms is responsible for the negative longitudinal piezoelectric effect. Building on these insights, it is predicted that, by controlling the environment of such active oxygens (e.g., by means of an epitaxial strain), it is possible to change the sign of the piezoelectric response of the material.

Probing Ferroelectric Behavior in Sub-10 nm Bismuth-Rich Aurivillius Films by Piezoresponse Force Microscopy

Sub-10 nm ferroelectric and multiferroic materials are attracting increased scientific and technological interest, owing to their exciting physical phenomena and prospects in miniaturized electronic devices, neuromorphic computing, and ultra-compact data storage. The Bi6Ti2.9Fe1.5Mn0.6O18 (B6TFMO) Aurivillius system is a rare example of a multiferroic that operates at room temperature. Since the formation of magnetic impurity phases can complicate attempts to measure ferromagnetic signal intrinsic to the B6TFMO multiferroic phase and thus limits its use, herein we minimize this by utilizing relatively large (49%) bismuth excess to counteract its volatility during sub-10 nm growth. X-ray diffraction, electron microscopy, and atomic force microscopy show sample crystallinity and purity are substantially improved on increasing bismuth excess from 5 to 49%, with the volume fraction of surface impurities decreasing from 2.95–3.97 vol% down to 0.02–0.31 vol%. Piezoresponse force microscopy reveals 8 nm B6TFMO films are ferroelectric, with an isotropic random distribution of stable in-plane domains and weaker out-of-plane piezoresponse. By reducing the volume fraction of magnetic impurities, this work demonstrates the recent progress in the optimization of ultra-thin B6TFMO for future multiferroic technologies. We show how the orientation of the ferroelectric polarization can be switched in 8 nm B6TFMO and arrays can be “written” and “read” to express states permitting anti-parallel information storage.

Cantilever signature of tip detachment during contact resonance AFM

Contact resonance atomic force microscopy, piezoresponse force microscopy, and electrochemical strain microscopy are atomic force microscopy modes in which the cantilever is held in contact with the sample at a constant average force while monitoring the cantilever motion under the influence of a small, superimposed vibrational signal. Though these modes depend on permanent contact, there is a lack of detailed analysis on how the cantilever motion evolves when this essential condition is violated. This is not an uncommon occurrence since higher operating amplitudes tend to yield better signal-to-noise ratio, so users may inadvertently reduce their experimental accuracy by inducing tip–sample detachment in an effort to improve their measurements. We shed light on this issue by deliberately pushing both our experimental equipment and numerical simulations to the point of tip–sample detachment to explore cantilever dynamics during a useful and observable threshold feature in the measured response. Numerical simulations of the analytical model allow for extended insight into cantilever dynamics such as full-length deflection and slope behavior, which can be challenging or unobtainable in a standard equipment configuration. With such tools, we are able to determine the cantilever motion during detachment and connect the qualitative and quantitative behavior to experimental features.

Screen Printed Copper and Tantalum Modified Potassium Sodium Niobate Thick Films on Platinized Alumina Substrates

We show how sintering in different atmospheres affects the structural, microstructural, and functional properties of ~30 μm thick films of K0.5Na0.5NbO3 (KNN) modified with 0.38 mol% K5.4Cu1.3Ta10O29 and 1 mol% CuO. The films were screen printed on platinized alumina substrates and sintered at 1100 °C in oxygen or in air with or without the packing powder (PP). The films have a preferential crystallographic orientation of the monoclinic perovskite phase in the [100] and [−101] directions. Sintering in the presence of PP contributes to obtaining phase-pure films, which is not the case for the films sintered without any PP notwithstanding the sintering atmosphere. The latter group is characterized by a slightly finer grain size, from 0.1 μm to ~2 μm, and lower porosity, ~6% compared with ~13%. Using piezoresponse force microscopy (PFM) and electron backscatter diffraction (EBSD) analysis of oxygen-sintered films, we found that the perovskite grains are composed of multiple domains which are preferentially oriented. Thick films sintered in oxygen exhibit a piezoelectric d33 coefficient of 64 pm/V and an effective thickness coupling coefficient kt of 43%, as well as very low mechanical losses of less than 0.5%, making them promising candidates for lead-free piezoelectric energy harvesting applications.

Formation of a quasi-equilibrium domain structure of crystals of the TGS group near TC

In the temperature range ΔT ≈ 321 K ÷ 322 K, the kinetics of the nonequilibrium domain structure of triglycine sulphate crystals, both pure and with specially introduced defects, has been studied by means of piezoresponse force microscopy technique. The temporal change in the domain structure as a set of regions with a scalar order parameter of P (r, t) = +1 and −1 for oppositely polarized domains was analysed by the behaviour of the space-time correlation function C(r,t) = ·Р(r,t)Р(0,t)Ò. At different distances from the Curie point Tc, the characteristic length Lc, as a scale measure of the average domain size, increases with time according to the power law Lc(t)~(t−t0)a. A decrease of the exponent a with distance from Tc can be a consequence of the transition of the domain structure of TGS crystals from a non-conservative state to aconservative one.

Symmetry-aware recursive image similarity exploration for materials microscopy

In pursuit of scientific discovery, vast collections of unstructured structural and functional images are acquired; however, only an infinitesimally small fraction of this data is rigorously analyzed, with an even smaller fraction ever being published. One method to accelerate scientific discovery is to extract more insight from costly scientific experiments already conducted. Unfortunately, data from scientific experiments tend only to be accessible by the originator who knows the experiments and directives. Moreover, there are no robust methods to search unstructured databases of images to deduce correlations and insight. Here, we develop a machine learning approach to create image similarity projections to search unstructured image databases. To improve these projections, we develop and train a model to include symmetry-aware features. As an exemplar, we use a set of 25,133 piezoresponse force microscopy images collected on diverse materials systems over five years. We demonstrate how this tool can be used for interactive recursive image searching and exploration, highlighting structural similarities at various length scales. This tool justifies continued investment in federated scientific databases with standardized metadata schemas where the combination of filtering and recursive interactive searching can uncover synthesis-structure-property relations. We provide a customizable open-source package (https://github.com/m3-learning/Recursive_Symmetry_Aware_Materials_Microstructure_Explorer) of this interactive tool for researchers to use with their data.