Electronic textiles and functional fabrics are among the key constituents envisioned for wearable electronics applications. For e‐textiles, the challenge is to process materials of desired electronic properties such as piezoelectricity into fibers to be integrated as wefts or wraps in the fabrics. Nylons, first introduced in the 1940s for stockings, are among the most widely used synthetic fibers in textiles. However, realization of nylon‐based e‐textiles has remained elusive due to the difficulty of achieving the piezoelectric phase in the nylon fibers. Here, piezoelectric nylon‐11 fibers are demonstrated and it is shown that the resulting fibers are viable for applications in energy harvesting from low frequency mechanical vibrations and in motion sensors. A simulation study is presented that elucidates on the sensitivity of the nylon‐11 fibers toward external mechanical stimuli. Moreover, a strategy is proposed and validated to significantly boost the electrical performance of the fibers. Since a large fraction of the textile industry is based on nylon fibers, the demonstration of piezoelectric nylon fibers will be a major step toward realization of electronic textiles for applications in apparels, health monitoring, sportswear, and portable energy generation.

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Ferroelectricity, a bistable ordering of electrical dipoles in a material, is widely used in sensors, actuators, nonlinear optics, and data storage. Traditional ferroelectrics are ceramic based. Ferroelectric polymers are inexpensive lead-free materials that offer unique features such as the freedom of design enabled by chemistry, the facile solution-based low-temperature processing, and mechanical flexibility. Among engineering polymers, odd nylons are ferroelectric. Since the discovery of ferroelectricity in polymers, nearly half a century ago, a solution-processed ferroelectric nylon thin film has not been demonstrated because of the strong tendency of nylon chains to form hydrogen bonds. We show the solution processing of transparent ferroelectric thin film capacitors of odd nylons. The demonstration of ferroelectricity, as well as the way to obtain thin films, makes odd nylons attractive for applications in flexible devices, soft robotics, biomedical devices, and electronic textiles.

Hierarchically porous piezoelectric polymer nanofibers are prepared through precise control over the thermodynamics and kinetics of liquid–liquid phase separation of nonsolvent (water) in poly(vinylidene fluoride‐trifluoroethylene) (P(VDF‐TrFE)) solution. Hierarchy is achieved by fabricating fibers with pores only on the surface of the fiber, or pores only inside the fiber with a closed surface, or pores that are homogeneously distributed in both the volume and surface of the nanofiber. For the fabrication of hierarchically porous nanofibers, guidelines are formulated. A detailed experimental and simulation study of the influence of different porosities on the electrical output of piezoelectric nanogenerators is presented. It is shown that bulk porosity significantly increases the power output of the comprising nanogenerator, whereas surface porosity deteriorates electrical performance. Finite element method simulations attribute the better performance to increased volumetric strain in bulk porous nanofibers.

Polymeric nanocomposite thin films of magnetic nanoparticles blended with the ferroelectric polymer poly-(vinylidene fluoride-co-trifluoroethylene) (P(VDF-TrFE)) are promising candidates for multiferroic applications. To date, only thick-film multiferroic nanocomposites have been reported. Fabrication of nanocomposite thin films along with the study of the ferroic properties with magnetic nanoparticle loading is crucial for the realization of functional devices. However, systematic studies, and in particular the dynamic of ferroelectric polarization switching and a solid understanding of the microstructure formation in thin films, are still missing. Here, we present solution-processed P(VDF-TrFE):magnetic nanoparticle thin films for multiferroic applications, wherein the ferroic properties, polarization switching dynamic, and the microstructure formation are studied as a function of nanoparticle loading. Our results demonstrate that as the nanoparticle loading increases, the ferroelectric polarization of the nanocomposite decreases and the saturation magnetization increases. Moreover, the presence of the nanoparticles substantially increases the polarization switching time and shifts the switching mechanism to one-dimensional growth. The P(VDF-TrFE):magnetic nanoparticle solution phase separates upon film casting. The crystalline regions of P(VDF-TrFE) are pure. The amorphous regions accommodate the nanoparticles. The phase separation leads to agglomerated nanoparticles at higher loadings, and eventually stratified vertical phases occur. The insight gained from the study of thin-film microstructure would help to optimize the performance of the nanocomposite for multiferroic applications and can be used for better understanding of the polymer:nanoparticle nanocomposites for energy storage and memory applications.

Despite the realization of ferroelectricity in the δ-phase of poly(vinyleden difluoride) (PVDF) nearly four decades ago, the dynamics of polarization switching has not been studied yet. Here, we unravel the polarization switching mechanism as a onedimensional process that is nucleated by a 90°rotation of a CH 2 −CF 2 repeat unit, forming a kink with reversed dipole along the polymer chain. The kink subsequently propagates in time, yielding full polarization reversal along the chain while preserving TGTG′ chain conformation. We show that the domain wall mobility in δ-phase PVDF is faster than both conventional ferroelectric β-phase PVDF and its copolymers with trifluoroethylene, P(VDF-TrFE). The switching time at infinite electric field for δ-phase PVDF is ten times faster and amounts to 500 ps. Fast switching dynamics combined with the low voltage operation and high thermal stability of polarization make δ-PVDF a suitable candidate for microelectronic applications.

Among odd‐nylons, nylon‐5 exhibits the highest remanent polarization and is thus a desirable material for many applications of ferroelectric polymers. However, nylon‐5 has never been used as a ferroelectric material, because the synthesis of nylon‐5 and its processing into thin films are challenging. This work revisits the synthesis of nylon‐5 via anionic ring opening polymerization (AROP) and studies the effect of reaction time and scale‐up on (i) molecular weight (Mn), (ii) melting point (Tm), (iii) yield, and (iv) ferroelectric properties. For the first time, the molecular weight of nylon‐5 is characterized via size exclusion chromatography (SEC), nuclear magnetic resonance (NMR) spectroscopy, as well as matrix assisted laser desorption ionization time of flight mass spectroscopy (MALDI ToF‐MS), showing Mn values of up to 12 500 g mol‐1. Extended reaction times and the synthesis on a larger scale increase the molecular weight and yield. Nylon‐5 thin films are fabricated from a TFA:acetone (60:40 mol%) solvent mixture. Nylon‐5 thin‐film capacitors are ferroelectric and show a remanent polarization as high as 12.5 ± 0.5 μC cm‐2, which is stable in time. The high remanent polarization values, combined with the facile solution processing, render nylon‐5 a promising candidate for future microelectronic and multi‐ferroic applications.

Organic bistable diodes based on phase-separated blends of ferroelectric and semiconducting polymers have emerged as promising candidates for non-volatile information storage for low-cost solution processable electronics. One of the bottlenecks impeding upscaling is stability and reliable operation of the array in air. Here, we present a memory array fabricated with an air-stable amine-based semiconducting polymer. Memory diode fabrication and full electrical characterizations were carried out in atmospheric conditions (23 °C and 45% relative humidity). The memory diodes showed on/off ratios greater than 100 and further exhibited robust and stable performance upon continuous write-read-erase-read cycles. Moreover, we demonstrate a 4-bit memory array that is free from cross-talk with a shelf-life of several months. Demonstration of the stability and reliable air operation further strengthens the feasibility of the resistance switching in ferroelectric memory diodes for low-cost applications.