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            Free, publicly-accessible full text available June 1, 2026
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            Free, publicly-accessible full text available March 1, 2026
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            A key component of cooling devices is the transfer of entropy from the cold load to heat sink. An electrocaloric (EC) polymer capable of generating both large electrocaloric effect (ECE) and substantial electroactuation can enable EC cooling devices to pump heat without external mechanisms, resulting in compact designs and enhanced efficiency. However, achieving both high ECE and significant electroactuation remains challenging. Herein, it is demonstrated that poly(vinylidene fluoride‐trifluoroethylene‐chlorofluoroethylene‐double bond) [P(VDF‐TrFE‐CFE‐DB)] tetrapolymers can simultaneously generate high electrocaloric effects and electroactuations under low fields. These P(VDF‐TrFE‐CFE‐DB) tetrapolymers are synthesized through the dehydrochlorination of P(VDF‐TrFE‐CFE) terpolymer. By facile tuning the composition of the initial terpolymer to avoid pure relaxor state, tetrapolymers with optimal DB compositions are achieved, near the critical endpoint of normal ferroelectric phase with diffused phase transition. The nearly vanishing energy barriers between the nonpolar to polar phases result in a strong electrocaloric response and significant electroactuation. Specifically, the P(VDF‐TrFE‐CFE‐DB) tetrapolymer exhibits an EC entropy change ΔSof 100 J kg−1 K−1under 100 MV m−1: comparable to state‐of‐the‐art (SOA) EC polymers, while delivering nearly twice the electroactuation of the SOA EC polymers. This work presents a general strategy for developing EC materials that combine large electrocaloric effect and electroactuation at low electric fields.more » « lessFree, publicly-accessible full text available June 1, 2026
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            Free, publicly-accessible full text available November 15, 2025
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            Abstract Interest in high‐entropy inorganic compounds originates from their ability to stabilize cations and anions in local environments that rarely occur at standard temperature and pressure. This leads to new crystalline phases in many‐cation formulations with structures and properties that depart from conventional trends. The highest‐entropy homogeneous and random solid solution is a parent structure from which a continuum of lower‐entropy offspring can originate by adopting chemical and/or structural order. This report demonstrates how synthesis conditions, thermal history, and elastic and chemical boundary conditions conspire to regulate this process in Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O, during which coherent CuO nanotweeds and spinel nanocuboids evolve. We do so by combining structured synthesis routes, atomic‐resolution microscopy and spectroscopy, density functional theory, and a phase field modeling framework that accurately predicts the emergent structure and local chemistry. This establishes a framework to appreciate, understand, and predict the macrostate spectrum available to a high‐entropy system that is critical to rationalizing property engineering opportunities.more » « lessFree, publicly-accessible full text available February 1, 2026
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            Spontaneous polarization as large as ∼28 μC/cm2 was recently observed around the dislocation cores in non-polar SrTiO3 bulk crystals, and its origin was attributed to the flexoelectric effect, i.e., polarization induced by strain gradients. However, the roles of flexoelectricity, relative to other electromechanical contributions, and the nature of dislocations, i.e., edge vs screw dislocations in the induced polarization, are not well understood. In this work, we study the role of flexoelectricity in inducing polarization around three types of dislocation cores in SrTiO3: b=a(100) edge dislocation, b=a(110) edge dislocation, and b=a(010) screw dislocation, where b is the Burgers vector. For the edge dislocations, polarization can be induced by electrostriction alone, while flexoelectricity is essential for stabilizing the symmetric polarization pattern. The shear component of the flexoelectric tensor has a dominant effect on the magnitude and spatial distribution of the flexoelectric polarization. In contrast, no polarization is induced around the b=a(010) screw dislocation through either electrostriction or flexoelectricity. Our findings provide an in-depth understanding of the role of flexoelectricity in inducing polarization around dislocation cores and offer insights into the defect engineering of dielectric/ferroelectric materials.more » « less
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