arXiv subjects

Eugene A. Eliseev

Publications and source records attributed to Eugene A. Eliseev.

At least 73 records · Page 4Linked to original sources

arXiv2022

Electric field control of labyrinth domain structures in core-shell ferroelectric nanoparticles

In the framework of the Landau-Ginzburg-Devonshire (LGD) approach, we studied the possibility of controlling the polarity and chirality of equilibrium domain structures by a homogeneous external electric field in a nanosized ferroelectric core covered with an ultra-thin shell of screening charge. Under certain screening lengths and core sizes, the minimum of the LGD energy, which consists of Landau-Devonshire energy, Ginzburg polarization gradient energy, and electrostatic terms, leads to the spontaneous appearance of stable labyrinth domain structures in the core. The labyrinths evolve from an initial polarization distribution consisting of arbitrarily small randomly oriented nanodomains. The equilibrium labyrinth structure is weakly influenced by details of the initial polarization distribution, such that one can obtain a quasi-continuum of nearly degenerate labyrinth structures, whose number is limited only by the mesh discretization density. Applying a homogeneous electric field to a nanoparticle with labyrinth domains, and subsequently removing it, allows inducing changes to the labyrinth structure, as the maze polarity is controlled by a field projection on the particle polar axis. Under specific conditions of the screening charge relaxation, the quasi-static dielectric susceptibility of the labyrinth structure can be negative, potentially leading to a negative capacitance effect. Considering the general validity of the LGD approach, we expect that an electric field control of labyrinth domains is possible in many spatially-confined nanosized ferroics, which can be potentially interesting for advanced cryptography and modern nanoelectronics.

cond-mat.mtrl-sci↗

arXiv2022

Hypothesis Learning in Automated Experiment: Application to Combinatorial Materials Libraries

Machine learning is rapidly becoming an integral part of experimental physical discovery via automated and high-throughput synthesis, and active experiments in scattering and electron/probe microscopy. This, in turn, necessitates the development of active learning methods capable of exploring relevant parameter spaces with the smallest number of steps. Here we introduce an active learning approach based on co-navigation of the hypothesis and experimental spaces. This is realized by combining the structured Gaussian Processes containing probabilistic models of the possible system's behaviors (hypotheses) with reinforcement learning policy refinement (discovery). This approach closely resembles classical human-driven physical discovery, when several alternative hypotheses realized via models with adjustable parameters are tested during an experiment. We demonstrate this approach for exploring concentration-induced phase transitions in combinatorial libraries of Sm-doped BiFeO3 using Piezoresponse Force Microscopy, but it is straightforward to extend it to higher-dimensional parameter spaces and more complex physical problems once the experimental workflow and hypothesis-generation are available.

cond-mat.mtrl-sci↗

arXiv2022

Size Effect of Local Current-Voltage Characteristics of MX$_2$ Nanoflakes: Local Density of States Reconstruction from Scanning Tunneling Microscopy Experiments

Local current-voltage characteristics for low-dimensional transition metal dichalcogenides (LD-TMD), as well as the reconstruction of their local density of states (LDOS) from scanning tunneling microscopy (STM) experiments is of fundamental interest and can be useful for advanced applications. Most of existing models are either hardly applicable for the LD-TMD of complex shape (e.g., those based on Simmons approach), or necessary for solving an ill-defined integral equation to deconvolute the unknown LDOS (e.g., those based on Tersoff approach). Using a serial expansion of Tersoff formulae, we propose a flexible method how to reconstruct the LDOS from local current-voltage characteristics measured in STM experiments. We established a set of key physical parameters, which characterize the tunneling current of a STM probe - sample contact and the sample LDOS expanded in Gaussian functions. Using a direct variational method coupled with a probabilistic analysis, we determine these parameters from the STM experiments for MoS2 nanoflakes with different number of layers. The main result is the reconstruction of the LDOS in a relatively wide energy range around a Fermi level, which allows insight in the local band structure of LD-TMDs. The reconstructed LDOS reveals pronounced size effects for the single-layer, bi-layer and three-layer MoS$_2$ nanoflakes, which we relate with low dimensionality and strong bending/corrugation of the nanoflakes. We hope that the proposed elaboration of the Tersoff approach allowing LDOS reconstruction will be of urgent interest for quantitative description of STM experiments, as well as useful for the microscopic physical understanding of the surface, strain and bending contribution to LD-TMDs electronic properties.

cond-mat.mtrl-sci↗

arXiv2022

Temperature-assisted Piezoresponse Force Microscopy: Probing Local Temperature-Induced Phase Transitions in Ferroics

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 contributions of the flexoelectric and thermopolarization effects to the local electromechanical response, and demonstrate that the latter can be significant for "soft" ferroelectrics. These results establish the framework for quantitative interpretation of tPFM observations, predict the emergence the non-trivial switching and relaxation phenomena driven by non-local thermal gradient-induced polarization switching, and open a pathway for exploring the physics of thermopolarization effects in various non-centrosymmetric and centrosymmetric materials.

cond-mat.mtrl-sci↗

arXiv2021

Chemical control of polarization in thin strained films of a multiaxial ferroelectric: phase diagrams and polarization rotation

The emergent behaviors in thin films of a multiaxial ferroelectric due to an electrochemical coupling between the rotating polarization and surface ions are explored within the framework of the 2-4 Landau-Ginzburg-Devonshire (LGD) thermodynamic potential combined with the Stephenson-Highland (SH) approach. The combined LGD-SH approach allows to describe the electrochemical switching and rotation of polarization vector in the multiaxial ferroelectric film covered by surface ions with a charge density dependent to the relative partial oxygen pressure. We calculate the phase diagrams and analyze the dependence of polarization components on the applied voltage, and discuss the peculiarities of quasi-static ferroelectric, dielectric and piezoelectric hysteresis loops in thin strained multiaxial ferroelectric films. The nonlinear surface screening by oxygen ions makes the diagrams very different from the known diagrams of e.g., strained BaTiO3 films. Quite unexpectedly we predict the appearance of the ferroelectric reentrant phases. Obtained results point on the possibility to control the appearance and features of ferroelectric, dielectric and piezoelectric hysteresis in multiaxial FE films covered by surface ions by varying their concentration via the partial oxygen pressure. The LGD-SH description of a multiaxial FE film can be further implemented within the Bayesian optimization framework, opening the pathway towards predictive materials optimization.

cond-mat.mtrl-sci↗

arXiv2021

Multi-objective Bayesian optimization of ferroelectric materials with interfacial control for memory and energy storage applications

Optimization of materials performance for specific applications often requires balancing multiple aspects of materials functionality. Even for the cases where generative physical model of material behavior is known and reliable, this often requires search over multidimensional parameter space to identify low-dimensional manifold corresponding to required Pareto front. Here we introduce the multi-objective Bayesian Optimization (MOBO) workflow for the ferroelectric/anti-ferroelectric performance optimization for memory and energy storage applications based on the numerical solution of the Ginzburg-Landau equation with electrochemical or semiconducting boundary conditions. MOBO is a low computational cost optimization tool for expensive multi-objective functions, where we update posterior surrogate Gaussian process models from prior evaluations, and then select future evaluations from maximizing an acquisition function. Using the parameters for a prototype bulk antiferroelectric (PbZrO3), we first develop a physics-driven decision tree of target functions from the loop structures. We further develop a physics-driven MOBO architecture to explore multidimensional parameter space and build Pareto-frontiers by maximizing two target functions jointly: energy storage and loss. This approach allows for rapid initial materials and device parameter selection for a given application and can be further expanded towards the active experiment setting. The associated notebooks provide both the tutorial on MOBO and allow to reproduce the reported analyses and apply them to other systems (https://github.com/arpanbiswas52/MOBO_AFI_Supplements).

cond-mat.mtrl-sci↗

arXiv2021

Chiral Polarization Textures Induced by the Flexoelectric Effect in Ferroelectric Nanocylinders

Polar chiral structures have recently attracted much interest within the scientific community, as they pave the way towards innovative device concepts similar to the developments achieved in nanomagnetism. Despite the growing interest, many fundamental questions related to the mechanisms controlling the appearance and stability of ferroelectric topological structures remain open. In this context, ferroelectric nanoparticles provide a flexible playground for such investigations. Here, we present a theoretical study of ferroelectric polar textures in a cylindrical core-shell nanoparticle. The calculations reveal a chiral polarization structure containing two oppositely oriented diffuse axial domains located near the cylinder ends, separated by a region with a zero-axial polarization. We name this polarization configuration "flexon" to underline the flexoelectric nature of its axial polarization. Analytical calculations and numerical simulation results show that the flexon's chirality can be switched by reversing the sign of the flexoelectric coefficient. Furthermore, the anisotropy of the flexoelectric coupling is found to critically influence the polarization texture and domain morphology. The flexon rounded shape, combined with its distinct chiral properties and the localization nature near the surface, are reminiscent of Chiral Bobber structures in magnetism. In the azimuthal plane, the flexon displays the polarization state of a vortex with an axially polarized core region, i.e., a meron. The flexoelectric effect, which couples the electric polarization and elastic strain gradients, plays a determining role in the stabilization of these chiral states. We discuss similarities between this interaction and the recently predicted ferroelectric Dyzaloshinskii-Moriya interaction leading to chiral polarization states.

cond-mat.mtrl-sci↗

arXiv2021

Effect of surface ionic screening on polarization reversal and phase diagrams in thin antiferroelectric films for information and energy storage

The emergent behaviors in antiferroelectric thin films due to a coupling between surface electrochemistry and intrinsic polar instabilities are explored within the framework of the modified 2-4-6 Kittel-Landau-Ginzburg-Devonshire (KLGD) thermodynamic approach. Using phenomenological parameters of the KLGD potential for a bulk antiferroelectric (PbZrO3) and a Stephenson-Highland (SH) approach, we study the role of surface ions with a charge density proportional to the relative partial oxygen pressure on the dipole states and their reversal mechanisms in the antiferroelectric thin films. The combined KLGD-SH approach allows to delineate the boundaries of antiferroelectric, ferroelectric-like antiferroionic and electret-like paraelectric states as a function of temperature, oxygen pressure, surface ions formation energy and concentration, and film thickness. This approach also allows the characterization of the polar and antipolar orderings dependence on the voltage applied to the antiferroelectric film, and the analysis of their static and dynamic hysteresis loops. The applications of the antiferroelectric films covered with surface ion layer for energy and information storage are explored.

cond-mat.mtrl-sci↗

arXiv2021

Flexo-Sensitive Polarization Vortices in Thin Ferroelectric Films

We consider theoretically the influence of the flexoelectric coupling on the spatial distribution and temperature behavior of spontaneous polarization for several types of stable domain structure in thin ferroelectric films, such as stripe domains and vortices.Finite element modelling (FEM) for BaTiO3 films and analytical calculations within the Landau-Ginzburg-Devonshire approach reveals that an out-of-plane polarization component can be very sensitive to the flexoelectric coupling for periodic quasi-2D stripe domains and 3D vortex-antivortex structures.However, the influence is rather different for these structures. The flexoelectric coupling increases significantly the amplitude of a small out-of-plane polarization component in the stripe domains, and the "up" or "down" direction of the component is defined by the sign of the flexoelectric coefficients.Concerning the vortex-antivortex pairs, their antivortices with in-plane anti-circulation have smooth wide dipolar cores through the entire film, whose shape and other features are almost insensitive to the coupling.The vortices with in-plane vorticity have spike-like cores with an out-of-plane quadrupolar moment induced by the flexoelectric coupling. The cores are located near the film-dead layer interfaces.FEM results corroborated by analytical calculations prove that a change of the flexoelectric coefficient sign leads to a reorientation of the core axial polarization, making the flexo-sensitive 3D vortices similar to the recently introduced "flexons" in cylindrical nanoparticles.The relatively wide temperature range (from 200 to 400 K) of the flexo-sensitive vortices' existence gives us the hope that they can be observed experimentally in thin ferroelectric films by scanning probe and nonlinear optical microscopy methods.

cond-mat.mtrl-sci↗

arXiv2021

Stress-Induced Phase Transitions in Nanoscale CuInP$_2$S$_6$

Using Landau-Ginsburg-Devonshire approach and available experimental results we reconstruct the thermodynamic potential of the layered ferroelectric CuInP$_2$S$_6$ (CIPS), which is expected to be applicable a wide range of temperatures and applied pressures. The analysis of temperature dependences of the dielectric permittivity and lattice constants for different applied pressures unexpectedly reveals the critically important role of the nonlinear electrostriction in this material. With the nonlinear electrostriction included we calculated temperature and pressure phase diagrams and spontaneous polarization of bulk CIPS. Using the coefficients of the reconstructed four-well thermodynamic potential, we study the strain-induced phase transitions in thin epitaxial CIPS films, as well as the stress-induced phase transitions in CIPS nanoparticles, which shape varies from prolate needles to oblate disks. We reveal the strong influence of the mismatch strain, elastic stress and shape anisotropy on the polar properties and phase diagrams of nanoscale CIPS. Also, we derived analytical expressions, which allow the elastic control of the nanoscale CIPS polar properties. Hence obtained results can be of particular interest for the strain-engineering of nanoscale layered nanoferroelectrics.

cond-mat.mtrl-sci↗

arXiv2021

Mapping causal patterns in crystalline solids

The evolution of the atomic structures of the combinatorial library of Sm-substituted thin film BiFeO3 along the phase transition boundary from the ferroelectric rhombohedral phase to the non-ferroelectric orthorhombic phase is explored using scanning transmission electron microscopy (STEM). Localized properties including polarization, lattice parameter, and chemical composition are parameterized from atomic-scale imaging and their causal relationships are reconstructed using a linear non-Gaussian acyclic model (LiNGAM). This approach is further extended toward exploring the spatial variability of the causal coupling using the sliding window transform method, which revealed that new causal relationships emerged both at the expected locations, such as domain walls and interfaces, but also at additional regions forming clusters in the vicinity of the walls or spatially distributed features. While the exact physical origins of these relationships are unclear, they likely represent nanophase separated regions in the morphotropic phase boundaries. Overall, we pose that an in-depth understanding of complex disordered materials away from thermodynamic equilibrium necessitates understanding not only of the generative processes that can lead to observed microscopic states, but also the causal links between multiple interacting subsystems.

physics.data-an↗

arXiv2021

A Combined Theoretical and Experimental Study of the Phase Coexistence and Morphotropic Boundaries in Ferroelectric-Antiferroelectric-Antiferrodistortive Multiferroics

The physical nature of the ferroelectric (FE), ferrielectric (FEI) and antiferroelectric (AFE) phases, their coexistence and spatial distributions underpin the functionality of antiferrodistortive (AFD) multiferroics in the vicinity of morphotropic phase transitions. Using Landau-Ginzburg-Devonshire (LGD) phenomenology and a semi-microscopic four sublattice model (FSM), we explore the behavior of different AFE, FEI and FE long-range orderings and their coexistence at the morphotropic phase boundaries in FE-AFE-AFD multiferroics. These theoretical predictions are compared with the experimental observations for dense Bi1-yRyFeO3 ceramics, where R is Sm or La atoms with the fraction 0 < y< 0.25, as confirmed by the X-ray diffraction (XRD) and Piezoresponse Force Microscopy (PFM). These complementary measurements were used to study the macroscopic and nanoscopic transformation of the crystal structure with the doping. The comparison of the measured and calculated AFE/FE phase fractions demonstrate that the LGD-FSM approach well describes the experimental results obtained by XRD and PFM for Bi1-yRyFeO3. Hence, this combined theoretical and experimental approach provides further insight into the origin of the morphotropic boundaries and coexisting FE and AFE states in model rare-earth doped multiferroics.

cond-mat.mtrl-sci↗

arXiv2021

Exploring physics of ferroelectric domain walls via Bayesian analysis of atomically resolved STEM data

The physics of ferroelectric domain walls is explored using the Bayesian inference analysis of atomically resolved STEM data. We demonstrate that domain wall profile shapes are ultimately sensitive to the nature of the order parameter in the material, including the functional form of Ginzburg-Landau-Devonshire expansion, and numerical value of the corresponding parameters. The preexisting materials knowledge naturally folds in the Bayesian framework in the form of prior distributions, with the different order parameters forming competing (or hierarchical) models. Here, we explore the physics of the ferroelectric domain walls in BiFeO3 using this method, and derive the posterior estimates of relevant parameters. More generally, this inference approach both allows learning materials physics from experimental data with associated uncertainty quantification, and establishing guidelines for instrumental development answering questions on what resolution and information limits are necessary for reliable observation of specific physical mechanisms of interest.

cond-mat.mtrl-sci↗

arXiv2020

Mesoscopic theory of defect ordering-disordering transitions in thin oxide films

Ordering of mobile defects in functional materials can give rise to fundamentally new phases possessing ferroic and multiferroic functionalities. Here we develop the Landau theory for strain induced ordering of defects (e.g. oxygen vacancies) in thin oxide films, considering both the ordering and wavelength of possible instabilities. Using derived analytical expressions for the energies of various defect-ordered states, we calculated and analyzed phase diagrams dependence on the film-substrate mismatch strain, concentration of defects, and Vegard coefficients. Obtained results open possibilities to create and control superstructures of ordered defects in thin oxide films by selecting the appropriate substrate and defect concentration.

cond-mat.mtrl-sci↗

arXiv2020

Flexo-Elastic Control Factors of Domain Morphology in Core-Shell Ferroelectric Nanoparticles: Soft and Rigid Shells

Within the framework of the Landau-Ginzburg-Devonshire approach we explore the impact of elastic anisotropy, electrostriction, flexoelectric couplings, and mismatch strain on the domain structure morphology in ferroelectric core-shell nanoparticles of spherical shape. We perform finite element modelling (FEM) for multiaxial ferroelectric nanoparticle cores covered with an elastically-isotropic soft or elastically-anisotropic rigid paraelectric shell, with and without mismatch strains. In the case of a core covered with a soft shell, the FEM results show that at room temperature a single polarization vortex with a dipolar kernel can be stable if the electrostriction coupling is weak. With increasing anisotropic electrostriction coupling, the vortex disappears and is replaced by complex flux-closure structures, which are formed in the equatorial plane and transform into an elongated vortex with a central 180-degree domain wall near the core poles. This complex domain morphology develops in the core due to the anisotropic electrostriction, and the flexoelectric coupling leads to an additional curvature and twist of the polarization isosurfaces. In contrast to this, FEM performed for a core covered with a rigid shell shows that, at room temperature, the anisotropic elastic properties of the shell can stabilize vortex-like structures with three flux-closure domains, which gradually cross in the equatorial plane of the core and transform into 120-degree domains near the core poles. The flexoelectric coupling leads to a noticeable curling of the flux-closure domain walls. A mismatch strain compensates the curling of the flux-closure domains in the core confined by the elastically-anisotropic rigid shell. Our analysis reveals different types of topological defects, namely Bloch point structures (BPS) and Ising lines, that form in a ferroelectric core covered with a soft or rigid shell.

cond-mat.mtrl-sci↗

arXiv2020

Correlation between corrugation-induced flexoelectric polarization and conductivity of low-dimensional transition metal dichalcogenides

Tunability of polar and semiconducting properties of low-dimensional transition metal dichalcogenides (TMDs) have propelled them to the forefront of fundamental and applied physical research. These materials can vary from non-polar to ferroelectric, and from direct-band semiconductor to metallic. However, in addition to classical controls such as composition, doping, and field effect in TMDs the additional degrees of freedom emerge due to the curvature-induced electron redistribution and associated changes in electronic properties. Here we numerically explore the elastic and electric fields, flexoelectric polarization and free charge density for a TMD nanoflake placed on a rough substrate with a sinusoidal profile of the corrugation using finite element modelling. Numerical results for different flake thickness and corrugation depth yield insight into the flexoelectric nature of the out-of-plane electric polarization and establish the unambiguous correlation between the polarization and static conductivity modulation caused by inhomogeneous elastic strains coupled with deformation potential and strain gradients, which evolve in TMD nanoflake due to the adhesion between the flake surface and corrugated substrate. We revealed a pronounced maximum at the thickness dependences of the electron and hole conductivity of MoS2 and MoTe2 nanoflakes placed on a metallic substrate, which opens the way for their geometry optimization towards significant improvement their polar and electronic properties, necessary for their advanced applications in nanoelectronics and memory devices.Specifically, obtained results can be useful for elaboration of nanoscale straintronic devices based on the bended MoS2, MoTe2 and MoSTe nanoflakes, such as diodes and bipolar transistors with a bending-controllable sharpness of p-n junctions.

cond-mat.mtrl-sci↗

arXiv2020

Phenomenological description of bright domain walls in ferroelectric-antiferroelectric layered chalcogenides

Recently, a layered ferroelectric CuInP2Se6 was shown to exhibit domain walls with locally enhanced piezoresponse - a striking departure from the observations of nominally zero piezoresponse in most ferroelectrics. Although it was proposed that such "bright" domain walls are phase-boundaries between ferri- and antiferroelectrically ordered regions of the materials, the physical mechanisms behind the existence and response of these boundaries remain to be understood. Here, using Landau-Ginzburg-Devonshire phenomenology combined with four sub-lattices model, we describe quantitatively the bright-contrast and dark-contrast domain boundaries between the antiferroelectric, ferroelectric or ferrielectric long-range ordered phases in a layered ferroelectric-antiferroelectric ferroics, such as CuInP2(S1-ySey)6

cond-mat.mtrl-sci↗

arXiv2020

Mesoscopic structure of mixed type domain walls in multiaxial ferroelectrics

The structure of 180-degree uncharged rotational domain wall in a multiaxial ferroelectric film is studied within the framework of analytical Landau-Ginzburg-Devonshire (LGD) approach. The Finite Element Modelling (FEM) is used to solve numerically the system of the coupled nonlinear Euler-Lagrange (EL) differential equations of the second order for two components of polarization. We show that the structure of the domain wall and corresponding (meta)stable phase of the film are controlled by a single master parameter, dimensionless ferroelectric anisotropy μ. We fitted the static profile of a solitary domain wall, calculated by FEM, with hyperbolic functions for polarization components, and extracted the five μ-dependent parameters from the fitting to FEM curves. The high accuracy of the fitting results allows us to conclude that the analytical functions can be treated as the high-accuracy variational solution of the static EL equations with cubic nonlinearity. We further derive the two-component analytical solutions of the static EL equations for a polydomain 180-degree domain structure in a multiaxial ferroelectric film. The analysis of the free energy dependence on the film thickness and boundary conditions at its surfaces allows to select the domain states corresponding to the minimal energy. The single-domain state is ground for zero polarization derivative at the surfaces, while the poly-domain states minimize the system energy for zero polarization at the surfaces. Counterintuitively, the energy of the polydomain states split into two levels 0 and 1 for zero polarization at the surfaces, and each of the levels is the infinite set of the close-energy sub-levels, which morphology is characterized by different structure of the two-component polarization nodes.

cond-mat.mtrl-sci↗