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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Giant Nonlinear Optical Response via Coherent Stacking of In-Plane Ferroelectric Layers

Thin ferroelectric materials hold great promise for compact nonvolatile memory and nonlinear optical and optoelectronic devices. Herein, an ultrathin in-plane ferroelectric material that exhibits a giant nonlinear optical effect, group-IV monochalcogenide SnSe, is reported. Nanometer-scale ferroelectric domains with ≈90°/270° twin boundaries or ≈180° domain walls are revealed in physical-vapor-deposited SnSe by lateral piezoresponse force microscopy. Atomic structure characterization reveals both parallel and antiparallel stacking of neighboring van der Waals ferroelectric layers, leading to ferroelectric or antiferroelectric ordering. Ferroelectric domains exhibit giant nonlinear optical activity due to coherent enhancement of second-harmonic fields and the as-resulted second-harmonic generation was observed to be 100 times more intense than monolayer WS 2 . This work demonstrates in-plane ferroelectric ordering and giant nonlinear optical activity in SnSe, which paves the way for applications in on-chip nonlinear optical components and nonvolatile memory devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Giant Domain Wall Conductivity in Self‐Assembled BiFeO 3 Nanocrystals

Abstract Ever‐increasing demand on electronic devices with ultrahigh‐density non‐volatile data storage has attracted great interest in novel ferroelectric memories based on conductive ferroelectric domain walls. Embedded in an insulating material, ferroelectric domain walls have the capability of being (re)created, displaced, erased, and altered in their spatial configurations and electronic characteristics. However, the domain wall conductivities are in most cases not yet sufficiently high to ensure the current density required to drive read‐out circuits operating at high speeds. In this work, a giant domain wall current (>10 µA) of a single charged domain wall is obtained through conductive atomic force microscopy with a bias field of 4 V. This is achieved in self‐assembled BiFeO 3 nanocrystals grown by sol‐gel method on Nb‐doped SrTiO 3 substrates. Local configurations of domains and domain wall types are studied using vector piezoresponse force microscopy and high‐resolution transmission electronic microscopy. The enhancement of the wall current is shown to be due to the formation of conducting pathways of charged defects accumulated along domain walls and traversing the nanocrystals. The diverse domain walls can be manipulated by electric field in a perpendicular architecture. The perpendicular array structure of BiFeO 3 nanocrystals should have great potentials for developing perpendicular nanoelectronic prototypes.

Liu, Lisha↗
DOE OSTI2024

Observation of Antiferroelectric Domain Walls in a Uniaxial Hyperferroelectric

Abstract Ferroelectric domain walls are a rich source of emergent electronic properties and unusual polar order. Recent studies show that the configuration of ferroelectric walls can go well beyond the conventional Ising‐type structure. Néel‐, Bloch‐, and vortex‐like polar patterns have been observed, displaying strong similarities with the spin textures at magnetic domain walls. Here, the discovery of antiferroelectric domain walls in the uniaxial ferroelectric Pb 5 Ge 3 O 11 is reported. Highly mobile domain walls with an alternating displacement of Pb atoms are resolved, resulting in a cyclic 180° flip of dipole direction within the wall. Density functional theory calculations show that Pb 5 Ge 3 O 11 is hyperferroelectric, allowing the system to overcome the depolarization fields that usually suppress the antiparallel ordering of dipoles along the longitudinal direction. Interestingly, the antiferroelectric walls observed under the electron beam are energetically more costly than basic head‐to‐head or tail‐to‐tail walls. The results suggest a new type of excited domain‐wall state, expanding previous studies on ferroelectric domain walls into the realm of antiferroic phenomena.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Freestanding Ferroelectric Bubble Domains

Bubble-like domains, typically a precursor to the electrical skyrmions, arise in ultrathin complex oxide ferroelectric-dielectric-ferroelectric heterostructures epitaxially clamped with flat substrates. Here, it is reported that these specially ordered electric dipoles can also be retained in a freestanding state despite the presence of inhomogeneously distributed structural ripples. By probing local piezo and capacitive responses and using atomistic simulations, this study analyzes these ripples, sheds light on how the bubbles are stabilized in the modified electromechanical energy landscape, and discusses the difference in morphology between bubbles in freestanding and as-grown states. Furthermore, these results are anticipated to be the starting point of a new paradigm for the exploration of electric skyrmions with arbitrary boundaries and physically flexible topological orders in ferroelectric curvilinear space.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Understanding nanoscale structural distortions in Pb(Zr 0.2 Ti 0.8 )O 3 by utilizing X-ray nanodiffraction and clustering algorithm analysis

Hard X-ray nanodiffraction provides a unique nondestructive technique to quantify local strain and structural inhomogeneities at nanometer length scales. However, sample mosaicity and phase separation can result in a complex diffraction pattern that can make it challenging to quantify nanoscale structural distortions. In this work, a k-means clustering algorithm was utilized to identify local maxima of intensity by partitioning diffraction data in a three-dimensional feature space of detector coordinates and intensity. This technique has been applied to X-ray nanodiffraction measurements of a patterned ferroelectric PbZr 0.2 Ti 0.8 O 3 sample. The analysis reveals the presence of two phases in the sample with different lattice parameters. A highly heterogeneous distribution of lattice parameters with a variation of 0.02 Å was also observed within one ferroelectric domain. This approach provides a nanoscale survey of subtle structural distortions as well as phase separation in ferroelectric domains in a patterned sample.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Asymmetric Character of the Ferroelectric Phase Transition and Charged Domain Walls in a Hybrid Improper Ferroelectric

Abstract In improper ferroelectrics, the spontaneous ordering is typically driven by a structural distortion or a magnetic spin alignment. The induced electric polarization is only a secondary effect. This dependence is a rich source for unusual phenomena and ferroelectric domain configurations for proper, polarization‐driven ferroelectrics. This study focuses on the polar domain structure and the hysteretic behavior at the ferroelectric phase transition in Ca 3 Mn 1.9 Ti 0.1 O 7 as a representative of the recently discovered hybrid improper ferroelectric class of multiferroics. Combining optical second harmonic generation and Raman spectroscopy gives access to the spontaneous structural distortion and the resulting improper electric polarization. This study shows that hybrid improper ferroelectrics contrast proper and improper ferroelectrics in several ways. Most intriguingly, adjacent ferroelectric domains favor head‐to‐head and tail‐to‐tail domain walls over charge‐neutral configurations. Furthermore, the phase transition occurs in an asymmetric fashion. The regime of phase coexistence of the nonpolar and polar phases shows a clear and abrupt upper temperature limit. In contrast, the coexistence toward low temperatures is best described as a fade‐out process, where 100‐nm‐sized islands of the nonpolar phase expand deep into the polar phase.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Polarization Switching on the Open Surfaces of the Wurtzite Ferroelectric Nitrides: Ferroelectric Subsystems and Electrochemical Reactivity

Binary ferroelectric nitrides are promising materials for information technologies and power electronics. However, polarization switching in these materials is highly unusual. From the structural perspective, polarization reversal is associated with the change of the effective polarity at the surfaces and interfaces from N‐to‐M terminated, suggesting strong coupling between ferroelectric and chemical phenomena. Phenomenologically, macroscopic studies demonstrate the presence of complex time dependent phenomena including wake‐up. Here, in this study, the polarization switching using the multidimensional high‐resolution piezoresponse force microscopy (PFM) and spectroscopy is explored, detecting both the evolution of induced ferroelectric domain, electromechanical response, and surface deformation during first‐order reversal curve measurements. The presence of two weakly coupled ferroelectric subsystems are demonstrated and the bias‐induced electrochemical reactivity. The observed behaviors are very similar to the recent studies of other wurtzite system but additionally include electrochemical reactivity, suggesting the universality of these behaviors for the wurtzite binary ferroelectrics. These studies suggest potential of high‐resolution multimodal PFM spectroscopies to resolve complex coupled polarization dynamics in materials. Furthermore, these PFM based studies are fully consistent with the recent electron microscopy observations of the shark‐teeth like ferroelectric domains in nitrides. Hence, it is believed that these studies establish the universal phenomenological picture of polarization switching in binary wurtzite.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Influence of oxygen vacancies on the domain wall stability in BiFeO 3

Oxygen vacancy is the most common type of point defects in functional oxides, and it is known to have profound influence on their properties. This is particularly true for ferroelectric oxides since their interaction with ferroelectric polarization often dictates the ferroelectric responses. Here, we study the influence of the concentration of oxygen vacancies on the stability of ferroelectric domain walls (DWs) in BiFeO 3 , a material with a relatively narrow bandgap among all perovskite oxides, which enables strong interactions among electronic charge carriers, oxygen vacancies, and ferroelectric domains. It is found that the electronic charge carriers in the absence of oxygen vacancies have essentially no influence on the spatial polarization distribution of the DWs due to their low concentrations. Upon increasing the concentration of oxygen vacancies, charge-neutral DWs with an originally symmetric polarization distribution symmetric around the center of the wall can develop a strong asymmetry of the polarization field, which is mediated by the electrostatic interaction between polarization and electrons from the ionization of oxygen vacancies. Strongly charged head-to-head DWs that are unstable without oxygen vacancies can be energetically stabilized in the off-stoichiometric BiFeO 3–δ with δ ~ 0.02 where ionization of oxygen vacancies provides sufficient free electrons to compensate the bound charge at the wall. Our results delineate the electrostatic coupling of the ionic defects and the associated free electronic charge carriers with the bound charge in the vicinity of neutral and charged DWs in perovskite ferroelectrics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Strain effects on stability of topological ferroelectric polar configurations in (PbTiO3) n /(SrTiO3) n superlattices

The (PbTiO3)n/(SrTiO3)n (PTO/STO) superlattice system has been shown to exhibit interesting topological phases (e.g., vortices and skyrmions) in addition to normal ferroelectric domain states. Existing studies are mostly focused on the dependence of topological polar distributions and properties of PTO/STO superlattice on its periodicity. Here, we study the strain effect on the topological phase transitions and ferroelectric domain structures employing phase-field simulations. We summarized in an isotropic strain (in-plane misfit strain along the x direction is equal to that along the y direction) periodicity phase diagram displaying the stability regions of different polar topological states, including normal ferroelectric twins, vortices, skyrmions, and mixtures of vortices and twins. We also analyzed the polarization configurations under anisotropic in-plane strains (in-plane misfit strain along the x direction is not equal to that along the y direction) and demonstrated that the strain anisotropy can be used to tune the directions of vortex arrays along either the [100] pc or [010] pc directions or labyrinth vortex arrays. This work offers guidance to manipulating polar structures in the PTO/STO superlattices via strain engineering.

Physics↗
DOE OSTI2020

Giant Superelastic Piezoelectricity in Flexible Ferroelectric BaTiO3 Membranes

Mechanical displacement in commonly used piezoelectric materials is typically restricted to linear or biaxial in nature and to a few percent of the material dimensions. Here in this paper, we show that free-standing BaTiO 3 membranes exhibit nonconventional electromechanical coupling. Under an external electric field, these superelastic membranes undergo controllable and reversible “sushi-rolling-like” 180° folding–unfolding cycles. This crease-free folding is mediated by charged ferroelectric domains, leading to giant >3.8 and 4.6 μm displacements for a 30 nm thick membrane at room temperature and 60 °C, respectively. Further increasing the electric field above the coercive value changes the fold curvature, hence augmenting the effective piezoresponse. Finally, it is found that the membranes fold with increasing temperature followed by complete immobility of the membrane above the Curie temperature, allowing us to model the ferroelectric domain origin of the effect.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Towards automating structural discovery in scanning transmission electron microscopy *

Abstract Scanning transmission electron microscopy is now the primary tool for exploring functional materials on the atomic level. Often, features of interest are highly localized in specific regions in the material, such as ferroelectric domain walls, extended defects, or second phase inclusions. Selecting regions to image for structural and chemical discovery via atomically resolved imaging has traditionally proceeded via human operators making semi-informed judgements on sampling locations and parameters. Recent efforts at automation for structural and physical discovery have pointed towards the use of ‘active learning’ methods that utilize Bayesian optimization with surrogate models to quickly find relevant regions of interest. Yet despite the potential importance of this direction, there is a general lack of certainty in selecting relevant control algorithms and how to balance a priori knowledge of the material system with knowledge derived during experimentation. Here we address this gap by developing the automated experiment workflows with several combinations to both illustrate the effects of these choices and demonstrate the tradeoffs associated with each in terms of accuracy, robustness, and susceptibility to hyperparameters for structural discovery. We discuss possible methods to build descriptors using the raw image data and deep learning based semantic segmentation, as well as the implementation of variational autoencoder based representation. Furthermore, each workflow is applied to a range of feature sizes including NiO pillars within a La:SrMnO 3 matrix, ferroelectric domains in BiFeO 3 , and topological defects in graphene. The code developed in this manuscript is open sourced and will be released at github.com/nccreang/AE_Workflows .

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Unexpected Giant Microwave Conductivity in a Nominally Silent BiFeO 3 Domain Wall

Nanoelectronic devices based on ferroelectric domain walls (DWs), such as memories, transistors, and rectifiers, have been shown in recent years. Practical high-speed electronics, on the other hand, usually demand operation frequencies in the gigahertz (GHz) regime, where the effect of dipolar oscillation is important. Herein, an unexpected giant GHz conductivity on the order of 10 3 S m -1 is observed in certain BiFeO 3 DWs, which is about 100 000 times greater than the carrier-induced direct current (dc) conductivity of the same walls. Surprisingly, the nominal configuration of the DWs precludes the alternating current (ac) conduction under an excitation electric field perpendicular to the surface. Theoretical analysis reflects that the inclined DWs are stressed asymmetrically near the film surface, whereas the vertical walls in a control sample are not. The resultant imbalanced polarization profile can then couple to the out-of-plane microwave fields and induce power dissipation, which is confirmed by the phase-field modeling. Since the contributions from mobile-carrier conduction and bound-charge oscillation to the ac conductivity are equivalent in a microwave circuit, the research on local structural dynamics may open a new avenue to implement DW nano-devices for radio-frequency applications.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Light–ferroelectric interaction in two-dimensional lead iodide perovskites

The unique physical properties of two-dimensional (2D) metal halide perovskites (MHPs) such as nonlinear optics, anisotropic charge transport, and ferroelectricity have made these materials promising candidates for multifunctional applications. Recently, fluorine derivatives such as 4,4-difluoropiperidinium lead iodide perovskite or (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 have shown strong ferroelectricity as compared to other 2D MHPs. Although it was previously addressed that the ferroelectricity in MHPs can be affected by illumination, the underlying physical mechanisms of light–ferroelectricity interaction in 2D MHPs are still lacking. Here, we explore the electromechanical responses in 4,4-(DFPD) 2 PbI 4 thin films using advanced scanning probe microscopy techniques revealing ferroelectric domain structures. In this work, hysteretic ferroelectric loops measured by contact-Kelvin probe force microscopy are dependent on domain structures under dark conditions, while ferroelectricity weakens under illumination. The X-ray diffraction patterns exhibit significant changes in preferential orientation of individual lattice planes under illumination. Particularly, the reduced intensity of the (1 1 1) lattice plane under illumination leads to transitioning from a ferroelectric to a paraelectric phase. The instability of positive ions, especially molecular organic cations, is observed under illumination by time-of-flight secondary ion mass spectrometry. The combination of crystallographic orientation and chemical changes under illumination clearly contributes to the origin of light–ferroelectricity interaction in 2D (4,4-DFPD, C 5 H 10 F 2 N) 2 PbI 4 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Switchable planar chirality and spin texture in highly ordered ferroelectric hybrid perovskite domains

Chiral organic-inorganic hybrid perovskites offer a promising platform for developing non-linear chiro-optical applications and chiral-induced spin selectivity. Here, we show that achiral hybrid perovskites that have highly ordered ferroelectric domains with orthogonal polarization exhibit planar chirality, as manifested by second harmonic generation with strong circular dichroism. Interestingly, the handedness of the second harmonic generation circular dichroism response can be alternatingly switched between orthogonally polarized domains and domain walls. To correlate the origin of planar chirality in these domains, atom-resolved atomic force microscopy is used to reveal distinct arrangements of atomic rows in these ferroelectric crystals that indicate planar symmetry breaking. Remarkably, a large SHG anisotropy factor of 0.41 is measured at the domain wall. Additionally, spatially resolved two-photon photoluminescence excitation measurement provide evidence of larger Rashba spin-splitting in these chiral ferroelectric domains compared to domain-free areas. Our discoveries of domain-dependent planar chirality and spin texture hold great promise for advancement of domain-specific chiro-optical applications.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Phase-field simulation of domain size effect on dielectric and piezoelectric responses in K 0.5 Na 0.5 NbO 3 epitaxial thin films with superdomain structures

Size effects of mesoscale ferroelectric domains on the macroscopic dielectric and piezoelectric responses in domain-engineered bulk piezocrystals have been extensively studied for more than two decades. However, less is known about the domain size effects in ferroelectric epitaxial thin films, especially for films consisting of low-symmetry ferroelectric phases and exhibits hierarchical superdomain structures. Herein, using phase-field simulations, we systemically evaluate the effective out-of-plane dielectric and piezoelectric coefficients, κ$^{*}_{33}$ and d$^{*}_{33}$, as a function of the domain periods for two types of superdomain structures in ferroelectric K 0.5 Na 0.5 NbO 3 epitaxial thin films. In one type of the superdomain structures, we find that more than 70% increase of κ$^{*}_{33}$ and nearly 20% increase of d$^{*}_{33}$ can be achieved by tuning the domain period by a few tens of nanometers. Dissimilar behaviors are found when the domain period varies along different lateral directions, suggesting anisotropic domain size effects in thin films. By analyzing the local dielectric and piezoelectric responses from each domain variants and domain walls, we reveal that the domain size effect is governed by the variation of out-of-plane polarization inside the domains. Moreover, we also demonstrate enhanced domain size effects by modulating the misfit strains and temperature to approach the polymorphic phase boundaries, suggesting tunability of the size effect by doping and strain engineering. Furthermore, our results reveal multimodal domain size dependence of dielectric and piezoelectric responses in low-symmetry ferroelectric epitaxial thin films, implying that domain size engineering can be used to tune macroscopic properties of thin-film ferroelectrics, similar to their bulk counterparts.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Domain patterns and super-elasticity of freestanding BiFeO 3 membranes via phase-field simulations

Super-elasticity of functional ferroelectric oxides offers promises for integrating ferroelectric films into flexible electronics. However, super-elastic deformation is a complex phenomenon related to possibly multiple concurrent mechanisms. Fundamentally understanding how multiple mechanisms contribute to the super-elasticity of ferroelectric oxides is crucial to realizing their potential flexible electronic applications. In this study, we employ phase-field simulations to model the dynamics of ferroelectric domain patterns of freestanding BiFeO 3 membranes to understand the origin of their super-elasticity under substantial bending deformation (5% strain). It is demonstrated that both a reversible Rhombohedral-Tetragonal (R-T) phase transition and a nearly reversible domain evolution of BiFeO 3 membranes contribute to accommodating the large deformation and thus their super-elasticity. The dynamics of domain evolution also reveal the formation of an exotic ferroelectric vortex and polarization rotation before the phase transition. We constructed a diagram of phases and domain patterns as a function of the membrane thickness and bending angle, which allows one to readily predict the emergence of T phase and ferroelectric vortex in bent BFO membranes. These results not only provide fundamental understanding of mesoscale super-elastic mechanisms but also reveal exotic domain states of ferroelectric membranes.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Dynamics of Thermally Driven Domain Transformation in Ferroelectric Thin Films

An important feature in ultrathin ferroelectric films is the spontaneous formation of nanoscale polarization domain patterns. Epitaxial strain can greatly increase the ferroelectric transition temperature such that films can be in the ferroelectric state during growth. On the other hand, depolarization fields compete with ferroelectricity in ultrathin films, and, consequently, the optimal domain configuration during growth is a moving target. Under these conditions it is readily possible for a grown film to be in a nonequilibrium domain configuration. As the energy landscape in the system is quite complex, the relaxation dynamics by which a system can evolve towards the true equilibrium configuration are also quite interesting. Here, to capture the details of this process we used Bragg-geometry x-ray photon correlation spectroscopy (XPCS), in which x-ray scattering speckle patterns contain the information from the domain arrangements inside the film. With modest heating (∼15⁢0 °C) domain relaxation from 𝑇 (tetragonal) to 𝑀 𝐶 (monoclinic) was observed in BaTiO 3 films grown on ultrathin ferroelectric PbTiO 3 layers. Two-time correlation analysis reveals fascinating details associated with sticking points and reversals in the process.

36 MATERIALS SCIENCE↗