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  1. Abstract Piezoelectric polymers hold great potential for various electromechanical applications, but only show low performance, with | d 33  | < 30 pC/N. We prepare a highly piezoelectric polymer ( d 33  = −62 pC/N) based on a biaxially oriented poly(vinylidene fluoride) (BOPVDF, crystallinity = 0.52). After unidirectional poling, macroscopically aligned samples with pure β crystals are achieved, which show a high spontaneous polarization ( P s ) of 140 mC/m 2 . Given the theoretical limit of P s,β  = 188 mC/m 2 for the neat β crystal, the high P s cannot be explained by the crystalline-amorphous two-phase model (i.e., P s,β  = 270 mC/m 2 ). Instead, we deduce that a significant amount (at least 0.25) of an oriented amorphous fraction (OAF) must be present between these two phases. Experimental data suggest that the mobile OAF resulted in the negative and high d 33 for the poled BOPVDF. The plausibility of this conclusion is supported by molecular dynamics simulations.
  2. Poly(vinylidene fluoride) (PVDF) and its random copolymers exhibit the most distinctive ferroelectric properties; however, their spontaneous polarization (60–105 mC m −2 ) is still inferior to those (>200 mC m −2 ) of the ceramic counterparts. In this work, we report an unprecedented spontaneous polarization ( P s = 140 mC m −2 ) for a highly poled biaxially oriented PVDF (BOPVDF) film, which contains a pure β crystalline phase. Given the crystallinity of ∼0.52, the P s for the β phase ( P s,β ) is calculated to be 279 mC m −2 , if a simple two-phase model of semicrystalline polymers is assumed. This high P s,β is invalid, because the theoretical limit of P s,β is 185 mC m −2 , as calculated by density functional theory. To explain such a high P s for the poled BOPVDF, a third component in the amorphous phase must participate in the ferroelectric switching to contribute to the P s . Namely, an oriented amorphous fraction (OAF) links the lamellar crystal and the mobile amorphous fraction. From the hysteresis loop study, the OAF content was determined to be ∼0.28, more than 50% of the amorphous phase. Because of the highmore »polarizability of the OAFs, the dielectric constant of the poled BOPVDF reached nearly twice the value of conventional PVDF. The fundamental knowledge obtained from this study will provide a solid foundation for the future development of PVDF-based high performance electroactive polymers for wearable electronics and soft robotic applications.« less
  3. High energy density, high temperature, and low loss polymer dielectrics are highly desirable for electric energy storage, e.g., film capacitors in the power electronics of electric vehicles and high-speed trains. Fundamentally, high polarization and low dielectric loss are two conflicting physical properties, because more polarization processes will involve more loss mechanisms. As such, we can only achieve a delicate balance between high dielectric constant and reasonably low loss. This review focuses on achieving low dielectric loss while trying to enhance dielectric constants for dielectric polymers, which can be divided into two categories: extrinsic and intrinsic. For extrinsic dielectric systems, the working mechanisms include dipolar (e.g., nanodielectrics) and space charge (e.g., ion gels) interfacial polarizations. These polarizations do not increase the intrinsic dielectric constants, but cause decreased breakdown strength and increased dielectric loss for polymers. For intrinsic dielectric polymers, the dielectric constant originates from electronic, atomic (or vibrational), and orientational polarizations, which are intrinsic to the polymers themselves. Because of the nature of molecular bonding for organic polymers, the dielectric constant from electronic and atomic polarizations is limited to 2-5 for hydrocarbon-based insulators (i.e., band gap > 4 eV). It is possible to use orientational polarization to enhance intrinsic dielectric constantmore »while keeping reasonably low loss. However, nonlinear ferroelectric switching in ferroelectric polymers must be avoided. Meanwhile, paraelectric polymers often exhibit high electronic conduction due to large chain motion in the paraelectric phase. In this sense, dipolar glass polymers are more attractive for low loss dielectrics, because frozen chain dynamics enables deep traps to prevent electronic conduction. Both side-chain and main-chain dipolar glass polymers are promising candidates. Furthermore, it is possible to combine intrinsic and extrinsic dielectric properties synergistically in multilayer films to enhance breakdown strength and further reduce dielectric loss for high dielectric constant polar polymers. At last, future research directions are briefly discussed for the ultimate realization of next generation polymer film capacitors.« less
  4. In response to the stringent requirements for future DC-link capacitors in electric vehicles (EVs), it is desirable to develop dielectric polymer films with high-temperature tolerance (at least 105 °C) and low loss (dissipation factor, tan δ < 0.003). Although the biaxially oriented poly(ethylene terephthalate) (BOPET) film has an alleged temperature rating of 120 °C, its dielectric performance in terms of breakdown strength and lifetime cannot satisfy the stringent requirements for power electronics in EVs. In this work, we carried out a structure–electrical insulation property relationship study to understand the working mechanism for various PET films, including a commercial BOPET film, an amorphous PET (AmPET) film, and two annealed PET films (AnPET, i.e., cold-crystallized from AmPET). Structural analyses revealed a uniform edge-on crystalline orientation in BOPET with the a* axis in the film normal direction. Meanwhile, a high content of the rigid amorphous fraction (RAF) was identified for BOPET, which resulted from biaxial stretching during processing. On the contrary, AnPET films had a random crystal orientation with lower RAF contents. From dielectric breakdown and lifetime studies, the high-crystallinity AnPET film exhibited better electrical insulation than BOPET, and AmPET had the worst electrical insulation. Electrical conductivity results revealed that the high RAF contentmore »in BOPET led to reasonably high breakdown strength and long lifetime only at low temperatures (<100 °C). Meanwhile, PET crystals were more insulating than the amorphous phase, whether mobile, rigid, or glassy. In particular, the flat-on lamellae in the AnPET film were more effective than the edge-on lamellae in BOPET in blocking the conduction of charge carriers (electrons and impurity ions). This understanding will help us design high-temperature semicrystalline polymer films for DC-link capacitors in EVs.« less
  5. High performance polymer dielectrics are a key component for printed electronics. In this work, organo-soluble polymers of intrinsic microporosity (PIMs) are reported for the first time to demonstrate desirable dielectric properties with a high permittivity (or κ ), heat resistance, and low dielectric loss simultaneously. Due to the highly dipolar sulfonyl side groups (4.5 D) and rigid contorted polymer backbone, a sulfonylated PIM (SO 2 -PIM) enabled friction-free rotation of sulfonyl dipoles in the nanopores. As such, an optimal balance between relatively high κ and low dielectric loss is achieved in a broad temperature window (−50–200 °C). For example, the discharged energy density reached 17 J cm −3 with κ = 6.0. The discharge efficiency was 94% at 150 °C/300 MV m −1 and 88% at 200 °C/200 MV m −1 . Furthermore, its application as a high- κ gate dielectric in field effect transistors (FETs) is demonstrated. With the bilayer SO 2 -PIM/SiO 2 gate dielectric, InSe FETs exhibited a high electron mobility in the range of 200–400 cm 2 V −1 s −1 , as compared to 40 cm 2 V −1 s −1 for the bare SiO 2 -gated InSe FET. This study indicates that highly dipolarmore »PIMs with a rigid polymer backbone and large free volume are promising as next generation gate dielectric materials for printed electronics.« less