The discovery of ultrahigh piezoelectricity in relaxor-ferroelectric solid solution single crystals is a breakthrough in ferroelectric materials. A key signature of relaxor-ferroelectric solid solutions is the existence of polar nanoregions, a nanoscale inhomogeneity, that coexist with normal ferroelectric domains. Despite two decades of extensive studies, the contribution of polar nanoregions to the underlying piezoelectric properties of relaxor ferroelectrics has yet to be established. Here we quantitatively characterize the contribution of polar nanoregions to the dielectric/piezoelectric responses of relaxor-ferroelectric crystals using a combination of cryogenic experiments and phase-field simulations. The contribution of polar nanoregions to the room-temperature dielectric and piezoelectric properties is in the range of 50–80%. A mesoscale mechanism is proposed to reveal the origin of the high piezoelectricity in relaxor ferroelectrics, where the polar nanoregions aligned in a ferroelectric matrix can facilitate polarization rotation. This mechanism emphasizes the critical role of local structure on the macroscopic properties of ferroelectric materials.

The demand for a new generation of high-temperature dielectric materials toward capacitive energy storage has been driven by the rise of high-power applications such as electric vehicles, aircraft, and pulsed power systems where the power electronics are exposed to elevated temperatures. Polymer dielectrics are characterized by being lightweight, and their scalability, mechanical flexibility, high dielectric strength, and great reliability, but they are limited to relatively low operating temperatures. The existing polymer nanocomposite-based dielectrics with a limited energy density at high temperatures also present a major barrier to achieving significant reductions in size and weight of energy devices. Here we report the sandwich structures as an efficient route to high-temperature dielectric polymer nanocomposites that simultaneously possess high dielectric constant and low dielectric loss. In contrast to the conventional single-layer configuration, the rationally designed sandwich-structured polymer nanocomposites are capable of integrating the complementary properties of spatially organized multicomponents in a synergistic fashion to raise dielectric constant, and subsequently greatly improve discharged energy densities while retaining low loss and high charge-discharge efficiency at elevated temperatures. At 150°C and 200 MV m −1 , an operating condition toward electric vehicle applications, the sandwich-structured polymer nanocomposites outperform the state-of-the-art polymer-based dielectrics in terms of energy density, power density, charge-discharge efficiency, and cyclability. The excellent dielectric and capacitive properties of the polymer nanocomposites may pave a way for widespread applications in modern electronics and power modules where harsh operating conditions are present.electrical energy storage | dielectric | polymer nanocomposites | capacitors | high temperature F ilm capacitors store electrical energy in dielectric materials in the form of an electrostatic field between two electrodes. They possess the highest power density (on the order of megawatts) and the best rate capability (on the order of microseconds) among the electrical energy storage devices and are critical for power electronics, power conditioning, and pulsed power applications (1-3). For instance, DC bus capacitors are essential components in the power inverters of electric vehicles for the conversion of direct current to alternating current, which is required to drive the vehicle's motor. Compared with ceramics, polymeric materials offer inherent advantages for capacitors, including their light weight, facile processability, scalability, high breakdown strength, and graceful failure mechanism (1-5). However, dielectric polymers often suffer from low operating temperatures, which fall short of the emerging demands for energy storage and conversion in harsh environments commonly present in automobile, aerospace power systems, and advanced microelectronics (6, 7). For example, to accommodate biaxially oriented polypropylen...

In order to increase the dielectric constants of polymer-based dielectrics, composite approaches, in which inorganic fillers with much higher dielectric constants are added to the polar polymer matrix, have been investigated. However, high dielectric constant fillers cause high local electric fields in the polymer, resulting in a large reduction of the electric breakdown strength. We show that a significant increase in the dielectric constant can be achieved in polyetherimide nanocomposites with nanofillers whose dielectric constant can be similar to that of the matrix. The presence of nanofillers reduces the constraints on the dipole response to the applied electric field, thus enhancing the dielectric constant. Our results demonstrate that through nanostructure engineering, the dielectric constant of nanocomposites can be enhanced markedly without using high dielectric constant nanofillers.

Fossil fuel internal combustion engines generate and release a huge amount of nitrogen dioxide, leading to respiratory and allergic diseases such as asthma, pneumonia, and possibly tuberculosis. Here we develop an alveolus-inspired membrane sensor (AIMS) for self-powered wearable nitrogen dioxide detection and personal physiological assessment. The bionic AIMS exhibits an excellent sensitivity up to 452.44%, a good linearity of 0.976, and superior selectivity under a NO2 concentration of 50 ppm. Furthermore, the AIMS can also be employed to diagnose human breath behaviors for breath analysis. The fundamental sensing mechanism is established using a combination of thermodynamic analysis, finite-element analysis, and phase-field simulations. It is found that the depolarization field inside the sensitive materials plays a crucial role in the self-powered gas-sensing performance. This work not only provides an efficient, low-cost, portable, and environmentally friendly means for active environmental assessment and personal biomonitoring but also provides a deep understanding of the gas-sensing mechanisms.

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Ferroelectric polymers have been regarded as the preferred matrix for high‐energy‐density dielectric polymer nanocomposites because of their highest dielectric constants among the known polymers. Despite a library of ferroelectric polymer‐based composites having been demonstrated as highly efficient in enhancing the energy density, the charge–discharge efficiency remains moderate because of the high intrinsic loss of ferroelectric polymers. Herein, a systematic study of the oxide nanofillers is presented with varied dielectric constants and the vital role of the dielectric match between the filler and the polymer matrix on the capacitive performance of the ferroelectric polymer composites is revealed. A combined experimental and simulation study is further performed to specifically investigate the effect of the nanofiller morphology on the electrica properties of the polymer nanocomposites. The solution‐processed ferroelectric polymer nanocomposite embedded with Al2O3 nanoplates exhibits markedly improved breakdown strength and discharged energy density along with an exceptional charge–discharge efficiency of 83.4% at 700 MV m−1, which outperforms the ferroelectric polymers and nanocomposites reported to date. This work establishes a facile approach to high‐performance ferroelectric polymer composites through capitalizing on the synergistic effect of the dielectric properties and morphology of the oxide fillers.

The tuning of functional properties in thick oxide films via nanoscaffolds induced large vertical lattice strain.

The electrocaloric effect (ECE) refers to conversion of thermal to electrical energy of polarizable materials and could form the basis for the next-generation refrigeration and power technologies that are highly efficient and environmentally friendly. Ferroelectric materials such as ceramic and polymer films exhibit large ECEs, but each of these monolithic materials has its own limitations for practical cooling applications. In this work, nanosized barium strontium titanates with systematically varied morphologies have been prepared to form polymer nanocomposites with the ferroelectric polymer matrix. The solution-processed polymer nanocomposites exhibit an extraordinary room-temperature ECE via the synergistic combination of the high breakdown strength of a ferroelectric polymer matrix and the large change of polarization with temperature of ceramic nanofillers. It is found that a sizable ECE can be generated under both modest and high electric fields, and further enhanced greatly by tailoring the morphology of the ferroelectric nanofillers such as increasing the aspect ratio of the nanoinclusions. The effect of the geometry of the nanofillers on the dielectric permittivity, polarization, breakdown strength, ECE and crystallinity of the ferroelectric polymer has been systematically investigated. Simulations based on the phase-field model have been carried out to substantiate the experimental results. With the remarkable cooling energy density and refrigerant capacity, the polymer nanocomposites are promising for solid-state cooling applications.