Ferroelectric Domain Wall Warp Memristor.

Domain walls are quasi-one-dimensional topological defects in ferroic materials, which can harbor emergent functionalities. In the case of ferroelectric domain wall (FEDW) devices, an exciting frontier has emerged: memristor-based information storage and processing approaches. Memristor solid-state FEDW devices presented thus far, however predominantly utilize a complex network of domain walls to achieve the desired regulation of density and charge state.

Motion and teleportation of polar bubbles in low-dimensional ferroelectrics.

Electric bubbles are sub-10nm spherical vortices of electric dipoles that can spontaneously form in ultra-thin ferroelectrics. While the static properties of electric bubbles are well established, little to nothing is known about the dynamics of these particle-like structures. Here, we reveal pathways to realizing both the spontaneous and controlled dynamics of electric bubbles in ultra-thin Pb(ZrTi)O films.

Magnetocapacitance at the Ni/BiInO Schottky Interface.

We report the observation of a magnetocapacitance effect at the interface between Ni and epitaxial nonpolar BiInO thin films at room temperature. A detailed surface study using X-ray photoelectron spectroscopy (XPS) reveals the formation of an intermetallic Ni-Bi alloy at the Ni/BiInO interface and a shift in the Bi 4f and In 3d core levels to higher binding energies with increasing Ni thickness. The latter infers band bending in BiInO, corresponding to the formation of a p-type Schottky barrier.

Ferroelectric solitons crafted in epitaxial bismuth ferrite superlattices.

In ferroelectrics, complex interactions among various degrees of freedom enable the condensation of topologically protected polarization textures. Known as ferroelectric solitons, these particle-like structures represent a new class of materials with promise for beyond-CMOS technologies due to their ultrafine size and sensitivity to external stimuli. Such polarization textures have scarcely been demonstrated in multiferroics.

Spherical ferroelectric solitons.

Spherical ferroelectric domains, such as electrical bubbles, polar skyrmion bubbles and hopfions, share a single and unique feature-their homogeneously polarized cores are surrounded by a vortex ring of polarization whose outer shells form a spherical domain boundary. The resulting polar texture, typical of three-dimensional topological solitons, has an entirely new local symmetry characterized by a high polarization and strain gradients. Consequently, spherical domains represent a different material system of their own with emergent properties drastically different from that of their surrounding medium.

Top-down patterning of topological surface and edge states using a focused ion beam.

The conducting boundary states of topological insulators appear at an interface where the characteristic invariant ℤ switches from 1 to 0. These states offer prospects for quantum electronics; however, a method is needed to spatially-control ℤ to pattern conducting channels. It is shown that modifying SbTe single-crystal surfaces with an ion beam switches the topological insulator into an amorphous state exhibiting negligible bulk and surface conductivity.

Effects of Multiple Local Environments on Electron Energy Loss Spectra of Epitaxial Perovskite Interfaces.

The role of local chemical environments in the electron energy loss spectra of complex multiferroic oxides was studied using computational and experimental techniques. The evolution of the O K-edge across an interface between bismuth ferrite (BFO) and lanthanum strontium manganate (LSMO) was considered through spectral averaging over crystallographically equivalent positions to capture the periodicity of the local O environments. Computational techniques were used to investigate the contribution of individual atomic environments to the overall spectrum, and the role of doping and strain was considered.

A Room-Temperature Ferroelectric Resonant Tunneling Diode.

Resonant tunneling is a quantum-mechanical effect in which electron transport is controlled by the discrete energy levels within a quantum-well (QW) structure. A ferroelectric resonant tunneling diode (RTD) exploits the switchable electric polarization state of the QW barrier to tune the device resistance. Here, the discovery of robust room-temperature ferroelectric-modulated resonant tunneling and negative differential resistance (NDR) behaviors in all-perovskite-oxide BaTiO /SrRuO /BaTiO QW structures is reported.

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.

Optical Tuning of Resistance Switching in Polycrystalline Gallium Phosphide Thin Films.

The nanoscale resistive switching characteristics of gallium phosphide (GaP) thin films directly grown on Si are investigated as a function of incident light. The formation of conductive channels along the grain boundaries is attributed to the presence of point defects and structural disorder, which provide the ideal environment to enable the filamentary switching process. Both first-principles calculations and UV-vis and photoluminescence spectroscopy strongly point to the possibility of mid-gap electronic states in the polycrystalline GaP film due to such defects.

Topology and control of self-assembled domain patterns in low-dimensional ferroelectrics.

Whilst often discussed as non-trivial phases of low-dimensional ferroelectrics, modulated polar phases such as the dipolar maze and the nano-bubble state have been appraised as essentially distinct. Here we emphasize their topological nature and show that these self-patterned polar states, but also additional mesophases such as the disconnected labyrinthine phase and the mixed bimeron-skyrmion phase, can be fathomed in their plurality through the unifying canvas of phase separation kinetics. Under compressive strain, varying the control parameter, i.

Large-scale multiferroic complex oxide epitaxy with magnetically switched polarization enabled by solution processing.

Complex oxides with tunable structures have many fascinating properties, though high-quality complex oxide epitaxy with precisely controlled composition is still out of reach. Here we have successfully developed solution-based single-crystalline epitaxy for multiferroic (1-)BiTiFe MgO-()CaTiO (BTFM-CTO) solid solution in large area, confirming its ferroelectricity at the atomic scale with strong spontaneous polarization. Careful compositional tuning leads to a bulk magnetization of 0.

Deterministic Ferroelastic Domain Switching Using Ferroelectric Bilayers.

Composition gradients, or dissimilar ferroelectric bilayers, demonstrate colossal electromechanical figures of merit attributed to the motion of ferroelastic domain walls. Yet, mechanistic understanding of polarization switching pathways that drive ferroelastic switching in these systems remains elusive. Here, the crucial roles of strain and electrostatic boundary conditions in ferroelectric bilayer systems are revealed, which underpin their ferroelastic switching dynamics.

Nondestructive Mapping of Long-Range Dislocation Strain Fields in an Epitaxial Complex Metal Oxide.

The misfit dislocations formed at heteroepitaxial interfaces create long-ranging strain fields in addition to the epitaxial strain. For systems with strong lattice coupling, such as ferroic oxides, this results in unpredictable and potentially debilitating functionality and device performance. In this work, we use dark-field X-ray microscopy to map the lattice distortions around misfit dislocations in an epitaxial film of bismuth ferrite (BiFeO), a well-known multiferroic.

Increase of power conversion efficiency in dye-sensitized solar cells through ferroelectric substrate induced charge transport enhancement.

Ferroelectric functionalized dye-sensitized solar cells were fabricated by using a positively-poled LiNbO substrate coated with ITO (ITO-LiNbO) as a collector electrode and demonstrated enhanced power conversion efficiency. Surface potential properties of TiO nanoparticle film coated on the ITO-LiNbO (TiO/ITO-LiNbO) examined by Kelvin probe force microscopy (KPFM) confirmed that a large electric field (a few 10 V/µm) generated from LiNbO can penetrate through the ITO layer and is applied to TiO film. This polarization-induced electric field leads to an increased photocurrent density by attracting and promoting electrons to direct transport through the mesoporous TiO network toward the collector electrode and a decreased charge recombination by facilitating electrons to pass through fewer boundaries of nanoparticles, resulting in high power conversion efficiency.

Nanoscale Bubble Domains and Topological Transitions in Ultrathin Ferroelectric Films.

Observation of a new type of nanoscale ferroelectric domains, termed as "bubble domains"-laterally confined spheroids of sub-10 nm size with local dipoles self-aligned in a direction opposite to the macroscopic polarization of a surrounding ferroelectric matrix-is reported. The bubble domains appear in ultrathin epitaxial PbZr Ti O /SrTiO /PbZr Ti O ferroelectric sandwich structures due to the interplay between charge and lattice degrees of freedom. The existence of the bubble domains is revealed by high-resolution piezoresponse force microscopy (PFM), and is corroborated by aberration-corrected atomic-resolution scanning transmission electron microscopy mapping of the polarization displacements.

In-situ observation of ultrafast 90° domain switching under application of an electric field in (100)/(001)-oriented tetragonal epitaxial Pb(ZrTi)O thin films.

Ferroelastic domain switching significantly affects piezoelectric properties in ferroelectric materials. The ferroelastic domain switching and the lattice deformation of both a-domains and c-domains under an applied electric field were investigated using in-situ synchrotron X-ray diffraction in conjunction with a high-speed pulse generator set up for epitaxial (100)/(001)-oriented tetragonal Pb(ZrTi)O (PZT) films grown on (100) SrRuO//(100)KTaO substrates. The 004 peak (c-domain) position shifts to a lower 2θ angle, which demonstrates the elongation of the c-axis lattice parameter of the c-domain under an applied electric field.

Nanoscale Probing of Elastic-Electronic Response to Vacancy Motion in NiO Nanocrystals.

Measuring the diffusion of ions and vacancies at nanometer length scales is crucial to understanding fundamental mechanisms driving technologies as diverse as batteries, fuel cells, and memristors; yet such measurements remain extremely challenging. Here, we employ a multimodal scanning probe microscopy (SPM) technique to explore the interplay between electronic, elastic, and ionic processes via first-order reversal curve I-V measurements in conjunction with electrochemical strain microscopy (ESM). The technique is employed to investigate the diffusion of oxygen vacancies in model epitaxial nickel oxide (NiO) nanocrystals with resistive switching characteristics.

Strain Dependent Electronic Structure and Band Offset Tuning at Heterointerfaces of ASnO (A=Ca, Sr, and Ba) and SrTiO.

The valence band (VB) electronic structure and VB alignments at heterointerfaces of strained epitaxial stannate ASnO (A=Ca, Sr, and Ba) thin films are characterized using in situ X-ray and ultraviolet photoelectron spectroscopies, with band gaps evaluated using spectroscopic ellipsometry. Scanning transmission electron microscopy with geometric phase analysis is used to resolve strain at atomic resolution. The VB electronic structure is strain state dependent in a manner that correlated with a directional change in Sn-O bond lengths with strain.

Universal Approach for Predicting Crystallography of Heterogeneous Epitaxial Nanocrystals with Multiple Orientation Relationships.

Heteroepitaxial nanocrystals are one of the most fundamentally and technologically important classes of materials systems. The correlation between form, dictated by crystallographic features such as growth habit and direction, and function, in terms of the ultimate physio-chemical properties is well established, thus placing an onus on precise synthesis control of nanocrystal morphology. Yet, nanocrystal heteroepitaxy can be a frustrating, time-consuming iterative process, particularly during the initial stages of development.

Nanoscale Origins of Ferroelastic Domain Wall Mobility in Ferroelectric Multilayers.

The nanoscale origins of ferroelastic domain wall motion in ferroelectric multilayer thin films that lead to giant electromechanical responses are investigated. We present direct evidence for complex underpinning factors that result in ferroelastic domain wall mobility using a combination of atomic-level aberration corrected scanning transmission electron microscopy and phase-field simulations in model epitaxial (001) tetragonal (T) PbZrTiO (PZT)/rhombohedral (R) PbZrTiO (PZT) bilayer heterostructures. The local electric dipole distribution is imaged on an atomic scale for a ferroelastic domain wall that nucleates in the R-layer and cuts through the composition breaking the T/R interface.

Direct evidence for the spin cycloid in strained nanoscale bismuth ferrite thin films.

Magnonic devices that utilize electric control of spin waves mediated by complex spin textures are an emerging direction in spintronics research. Room-temperature multiferroic materials, such as bismuth ferrite (BiFeO3), would be ideal candidates for this purpose. To realize magnonic devices, a robust long-range spin cycloid with well-known direction is desired, since it is a prerequisite for the magnetoelectric coupling.

Robust polarization and strain behavior of Sm-modified BiFeO3 piezoelectric ceramics.

The route to phase-pure BiFeO3 (BFO) ceramics with excellent ferroelectric and electromechanical properties is severely impeded by difficulties associated with the perovskite phase stability during synthesis. This has meant that dopants and solid solutions with BFO have been investigated as a means of not only improving the functional properties, but also of improving the perovskite phase formation of BFO-based ceramics. The present work focuses on Sm-modified BFO ceramics of composition Bi0.

Higher order harmonic detection for exploring nonlinear interactions with nanoscale resolution.

Nonlinear dynamics underpin a vast array of physical phenomena ranging from interfacial motion to jamming transitions. In many cases, insight into the nonlinear behavior can be gleaned through exploration of higher order harmonics. Here, a method using band excitation scanning probe microscopy (SPM) to investigate higher order harmonics of the electromechanical response, with nanometer scale spatial resolution is presented.

A template and catalyst-free metal-etching-oxidation method to synthesize aligned oxide nanowire arrays: NiO as an example.

Although NiO is one of the canonical functional binary oxides, there has been no report so far on the effective fabrication of aligned single crystalline NiO nanowire arrays. Here we report a novel vapor-based metal-etching-oxidation method to synthesize high-quality NiO nanowire arrays with good vertical alignment and morphology control. In this method, Ni foils are used as both the substrates and the nickel source; NiCl(2) powder serves as the additional Ni source and provides Cl(2) to initiate mild etching.