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Reducing the switching energy of ferroelectric thin films remains an important goal in the pursuit of ultralow-power ferroelectric memory and logic devices. Here, we elucidate the fundamental role of lattice dynamics in ferroelectric switching by studying both freestanding bismuth ferrite (BiFeO3) membranes and films clamped to a substrate. We observe a distinct evolution of the ferroelectric domain pattern, from striped, 71° ferroelastic domains (spacing of ~100 nm) in clamped BiFeO3 films, to large (10's of micrometers) 180° domains in freestanding films. By removing the constraints imposed by mechanical clamping from the substrate, we can realize a ~40% reduction of the switching voltage and a consequent ~60% improvement in the switching speed. Our findings highlight the importance of a dynamic clamping process occurring during switching, which impacts strain, ferroelectric, and ferrodistortive order parameters and plays a critical role in setting the energetics and dynamics of ferroelectric switching.

HfO2‐based ferroelectrics offer promises for next‐generation nonvolatile nanoscale devices owing to excellent CMOS compatibility and robust ferroelectricity at the nanoscale. However, fundamentally understanding the mechanism of polarization reversal and domain dynamics is challenging because the role of the spacer layer at the domain level in HfO2‐based ferroelectrics remains elusive. Here, it is realized that visualization of time‐resolved dynamics of nanoscale domain configurations in the epitaxial Hf0.5Zr0.5O2 thin films using phase‐field simulations. Scale‐free domain independent switchability (namely, irreducible stable polar domain down to 1 nm lateral size) and sharp domain walls that originate from weak interactions between adjacent domains characterized by the reduced gradient energy coefficient, which unravels the mesoscale mechanism of spacer layer in domain dynamics are demonstrated. Meanwhile, it is revealed that 180° polarization switching is dominated by the nucleation of a new domain with a high nucleation density, well described by the nucleation‐limited switching model. This study not only provides a fundamental mesoscale mechanism of the spacer layer, but also stimulates further studies on the manipulation of ultra‐scaled single domain state for designing high‐density and fast‐speed HfO2‐based ferroelectric memory. [ABSTRACT FROM AUTHOR]

Fluorite-structured HfO2 ferroelectrics exhibit remarkable ferroelectricity owing to the robust thickness scalability, rendering them promising for next-generation ferroelectric memories. Unlike the well-understood perovskite structured ferroelectrics, such as Pb(Zr,Ti)O3, the origin of ferroelectricity in HfO2 remains elusive, which impedes the experimental fabrication of pure and stable ferroelectric orthorhombic phase in films. This study seeks to elucidate its origin by analyzing the covalent nature of local chemical bonding and changes in orbital hybridization and by catching the typical feather of the half-unit-cell spacer/polar layer in the orthorhombic phase. Notably, we find that the differences in the hybridization intensity of the 2s orbitals of two types of O atoms (OI and OII) and 5d orbitals of Hf atoms play a crucial role in inducing ferroelectric distortion. Furthermore, we demonstrate that the intrinsic mechanisms of stress in enhancing the ferroelectricity of HfO2 originate from the modulation of orbital hybridization intensity of the Hf–O bonds. These insights provide a vital theoretical foundation for further exploration of ferroelectric phase transitions and property modulation in HfO2 and similar fluorite-structured ferroelectrics. [ABSTRACT FROM AUTHOR]

Polar vortex domains have recently become an emergent research field due to the abundant physical phenomena and potential applications in high-density memories. Here, we explore the mechanisms of creating polar vortex domains in the BiFeO3 (BFO) membranes subjected to different boundary conditions using phase-field simulations. A major difference is that the vortex in membrane can be stabilized even under short-circuit electrical boundary conditions compared to vortex in other systems, such as thin film or superlattice. We found that (a) the formation of polar vortex domains at the membrane interior under bending is mainly driven by the reduction of elastic energy under short-circuit boundary condition, and the vortex chirality (namely, clockwise and counterclockwise) could be identified by n-shape and u-shape bending; (b) in the unbent open-circuit BFO membrane case, exotic trapezoid-shaped vortex nanodomains form at the terminations of 109° domain walls (DWs) and partially charged 71° DWs, which is driven by the local depolarization field and the interplay among electrostatic, elastic, and gradient and Landau energies. We also examine Kittel's law by establishing the dependence of vortex periods on the membrane thickness. These results give further understanding of the effect of boundary conditions on the formation of polar vortex domains, guiding experimental designs of vortex-based high-density memories. [ABSTRACT FROM AUTHOR]

Low-dimensional ferroelectric topological textures show abundant configurations such as flux-closure quadrants and vortices, suggesting potential applications in nano-electronic devices. However, the deterministic control of those polar textures is still challenging. By using piezoresponse force microscopy, threefold or fourfold vertex domain structures were observed in self-assembled BiFeO3 nano-islands, and the formation of such polar topological textures is strongly dependent on the size and shape of the nano-island. Furthermore, the vertex domain textures confined by geometry can be reversibly switched back and forth by external electric field, which are stabilized by the competition between elastic energy and electrostatic energy. Stable threefold or fourfold vertex domain structures are formed on BiFeO3 nano-islands, depending on the size and shape of the nanoisland. [ABSTRACT FROM AUTHOR]

It has been known that ferroelectric charged domain walls (CDWs), which break the polarization continuity, may be electrically active with an elevated conductivity. However, the bound charge at CDWs may render them energetically unstable, and thus, forming CDWs naturally and manipulating them electrically is still challenging. Here, we theoretically utilize phase-field simulations to design spontaneously generated CDWs with center-type quad-domains in a single square-shaped BiFeO3 nanoisland. It is shown that the stability of the spontaneously emerging head-to-head domain walls with center-convergent quad-domains is mainly determined by three contributions, namely, the geometrical constraint from approximately 45°-tilted bottom edges, the electric boundary condition, and the necessary screening free charges to compensate head-to-head domain walls. It is demonstrated that the center-convergent quad-domains with head-to-head CDWs can be electrically switched to the center-divergent one with tail-to-tail CDWs, providing guidance for achieving ferroelectric domain-wall-based nanodevices with low-power dissipation. [ABSTRACT FROM AUTHOR]

Voltage controlled 180° magnetization reversal has been achieved in BiFeO3-based multiferroic heterostructures, which is promising for the future development of low-power spintronic devices. However, all existing reports involve the use of an in-plane voltage that is unfavorable for practical device applications. Here, we investigate, using phase-field simulations, the out-of-plane (i.e., perpendicular to heterostructures) voltage controlled magnetism in heterostructures consisting of CoFe nanodots and (110) BiFeO3 thin film or island. It is predicted that the in-plane component of the canted magnetic moment at the CoFe/BiFeO3 interface can be reversed repeatedly by applying a perpendicular voltage across the bottom (110) BiFeO3 thin film, which further leads to an in-plane magnetization reversal in the overlaying CoFe nanodot. The non-volatility of such perpendicular voltage controlled magnetization reversal can be achieved by etching the continuous BiFeO3 film into isolated nanoislands with the same in-plane sizes as the CoFe nanodot. The findings would provide general guidelines for future experimental and engineering efforts on developing the electric-field controlled spintronic devices with BiFeO3-based multiferroic heterostructures. [ABSTRACT FROM AUTHOR]

Polar domain walls in centrosymmetric ferroelastics induce inhomogeneity that is the origin of advantageous multifunctionality. In particular, polar domain walls promote charge-carrier separation and hence are promising for energy conversion applications that overcome the hurdles of the rate-limiting step in the traditional photoelectrochemical water splitting processes. Yet, while macroscopic studies investigate the materials at the device scale, the origin of this phenomenon in general and the emergence of polar domain walls during the structural phase transition in particular has remained elusive, encumbering the development of this attractive system. Here, it is demonstrated that twin domain walls arise in centrosymmetric BiVO 4 films and they exhibit localized piezoelectricity. It is also shown that during the structural phase transition from the tetragonal to monoclinic, the symmetry reduction is accompanied by an emergence of strain gradient, giving rise to flexoelectric effect and the polar domain walls. These results not only expose the emergence of polar domain walls at centrosymmetric systems by means of direct observation, but they also expand the realm of potential application of ferroelastics, especially in photoelectrochemistry and local piezoelectricity., (© 2022 Wiley-VCH GmbH.)