Entangled polarizations in ferroelectrics: A focused review of polar topologies

Precise manipulation of van der Waals forces within two-dimensional atomic layers allows for exact control over electron-phonon coupling, leading to the exceptional quantum properties. However, applying this technique to diverse structures such as three-dimensional materials is challenging. Therefore, investigating new hierarchical structures and different interlayer forces is crucial for overcoming these limitations and discovering novel physical properties. In this work, a multi-shelled ferromagnetic material with controllable shell numbers is developed. By strategically regulating the magnetic interactions between these shells, the magnetic properties of each shell are fine-tuned. This approach reveals distinctive magnetic characteristics including regulated magnetic domain configurations and enhanced effective fields. The nanoscale magnetic interactions between the shells were observed and analyzed, which shed light on the modified magnetic properties of each shell, enhancing the understanding and control of ferromagnetic materials. The distinctive magnetic interaction significantly boosts electromagnetic absorption at low-frequency frequencies used by fifth-generation (5G) wireless devices, outperforming ferromagnetic materials without multilayer structures by several folds. The application of magnetic interactions in materials science reveals thrilling prospects for technological and electronic innovation. This article is protected by copyright. All rights reserved.

Visualizing Nanoscale Interlayer Magnetic Interactions and Unconventional Low-Frequency Behaviors in Ferromagnetic Multi-shelled Structures.

Synthesis and structural properties of PbTiO_3 nanotube arrays using a TiO_2 template-assisted hydrothermal method

Abstract The discovery of polar vortices and skyrmions in ferroelectric‐dielectric superlattices [such as (PbTiO 3 ) n /(SrTiO 3 ) n ] has ushered in an era of novel dipolar topologies and corresponding emergent phenomena. The key to creating such emergent features has generally been considered to be related to counterpoising strongly polar and non‐polar materials thus creating the appropriate boundary conditions. This limits the utility these materials can have, however, by rendering (effectively) half of the structure unresponsive to applied stimuli. Here, using advanced thin‐film deposition and an array of characterization and simulation approaches, polar vortices are realized in all‐ferroelectric trilayers, multilayers, and superlattices built from the fundamental building block of (PbTiO 3 ) n /(Pb x Sr 1− x TiO 3 ) n wherein in‐plane ferroelectric polarization in the Pb x Sr 1− x TiO 3 provides the appropriate boundary conditions. These superlattices exhibit substantially enhanced electromechanical and ferroelectric responses in the out‐of‐plane direction that arise from the ability of the polarization in both layers to rotate to the out‐of‐plane direction under field. In the in‐plane direction, the layers are found to be strongly coupled during switching and when heterostructured with ferroelectric‐dielectric building blocks, it is possible to produce multistate switching. This approach expands the realm of systems supporting emergent dipolar texture formation and does so with entirely ferroelectric materials thus greatly improving their responses. 

Highly Responsive Polar Vortices in All‐Ferroelectric Heterostructures

Pb1-xSrxTiO3 solid solutions have been utilized to compositionally tune the phase transitions and ferroelectric properties and thus are attractive for potential applications in tunable microwave devices and pyroelectric energy harvesters. However, a reliable thermodynamic description of the Pb1-xSrxTiO3 system is currently lacking. Here, we establish a thermodynamic free energy density function for the Pb1-xSrxTiO3 solid solution system taking into account both the polarization and octahedral tilt, and validated it by reproducing the experimentally measured polarization, lattice parameters, and dielectric constant values. Based on the thermodynamic model, we successfully explain the experimentally observed dielectric anomalies by analyzing the interactions between ferroelectric and octahedral tilt order parameters and constructed a comprehensive temperature-composition Pb1-xSrxTiO3 phase diagram which can be used to guide future experimental synthesis and thin film growth. The thermodynamic model developed in this work can be employed not only to predict the ferroelectric and structural states and their properties for compositions that have not yet been synthesized but also used as input to model the formation of mesoscale domain structures using the phase-field method. 

Thermodynamics and Ferroelectric Properties of Pb1-xSrxTiO3 Solid Solutions

Ferroelectric nanotubes offer intriguing opportunities for stabilizing exotic polarization domains and achieving new or enhanced functionalities by tailoring the complex interplay among the geometry, surface effects, crystal symmetry, and more. Here, phase‐field simulations to predict the room‐temperature equilibrium polarization domain structure in (001)pc PbZr0.52Ti0.48O3 (PZT) nanotubes are used (pseudocubic (pc)). The simulations incorporate the influence of surface‐tension‐induced strains, which have been ignored in existing computational studies. It is found that (001)pc PZT nanotubes can host a unique class of topological polarization domain structures comprising non‐planar flux‐closures and anti‐flux‐closures that are inaccessible with ferroelectrics of planar geometry (e.g., thin‐films, nanodots). It is shown that surface‐tension‐induced strain is significantly enhanced in thin‐walled nanotubes and thereby can lead to noticeable modulation of the flux closures. Domain stability map as a function of the nanotube wall thickness and height is established. The results provide a basis for geometrical engineering of domain structures and associated functional (e.g., piezoelectric, electrocaloric) responses in ferroelectric nanotubes.

Geometric Control of Domain Structure Stability in Ferroelectric Nanotubes

Incorporating rare-earth elements into wurtzite nitride semiconductors, such as scandium-alloyed aluminum nitride (ScAlN), significantly enhances the piezoelectric response, which is vital for a broad range of acoustic, electronic, photonic, and quantum applications. To date, however, the measured piezoelectric response of nitride semiconductors is far below what theory has predicted. Herein, we demonstrate a simple, scalable, post-growth thermal annealing process that can dramatically boost the piezoelectric response of ScAlN. We achieve a 3.5-fold increase in the piezoelectric modulus, d33 for ScAlN, from 12.3 pC/N in the as-grown state to 45.5 pC/N, which is eight times larger than that of AlN commercially used in 5 G cellphones. The observed enhancement is unambiguously confirmed by three separate measurement techniques. Detailed material characterization techniques reveal that optimized annealing conditions significantly improve the macroscopic structural quality, achieving a more homogeneous and ordered domain orientation, and reduces the lattice parameter ratio (c/a) in the wurtzite crystal structure. The dramatic enhancement of d33 in ScAlN thin films promises extreme frequency scaling opportunities for bulk acoustic wave resonators for beyond-5 G applications. The authors present a process that boosts the piezoelectric properties of ScAlN thin films by 3.5 times, enhancing their performance for use in acoustic devices. The technique is scalable, cost effective, and could enable advanced sensors, clocks, and communication technologies.

Unprecedented enhancement of piezoelectricity of wurtzite nitride semiconductors via thermal annealing

Thermodynamic energy density function for quantum paraelectric KTaO3

Interlayer coupling in materials, such as exchange interactions at the interface between an antiferromagnet and a ferromagnet, can produce exotic phenomena not present in the parent materials. While such interfacial coupling in magnetic systems has been widely studied, there is considerably less work on analogous electric counterparts (i.e., akin to electric "exchange-bias-like" or "exchange-spring-like" interactions between two polar materials) despite the likelihood that such effects could also engender new features associated with anisotropic electric dipole alignment. Here, electric analogs of such exchange interactions are reported, and their physical origins are explained for bilayers of in-plane polarized Pb1-x Srx TiO3 ferroelectrics. Variation of the strontium content and thickness of the layers provides for deterministic control over the switching properties of the bilayer system resulting in phenomena analogous to an exchange-spring interaction and, leveraging added control of these interactions with an electric field, the ability to realize multistate-memory function. Such observations not only hold technological promise for ferroelectrics and multiferroics, but also extend the similarities between ferromagnetic and ferroelectric materials to include the manifestation of exchange-interaction-like phenomena. This article is protected by copyright. All rights reserved.

Exchange-Interaction-Like Behavior in Ferroelectric Bilayers.

pdf/thermodynamic-theory-of-linear-optical-and-electro-optical-967pgi72ky0q.pdf

Thermodynamic theory of linear optical and electro-optical properties of ferroelectrics

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