Although traditional materials discovery has historically benefited from intuition-driven experimental approaches and serendipity, computational strategies have risen in prominence and proven to be a powerful complement to experiments in the modern materials research environment. It is illustrated here how one may harness a rational co-design approach-involving synergies between high-throughput computational screening and experimental synthesis and testing-with the example of polymer dielectrics design for electrostatic energy storage applications. Recent co-design efforts that can potentially enable going beyond present-day "standard" polymer dielectrics (such as biaxially oriented polypropylene) are highlighted. These efforts have led to the identification of several new organic polymer dielectrics within known generic polymer subclasses (e.g., polyurea, polythiourea, polyimide), and the recognition of the untapped potential inherent in entirely new and unanticipated chemical subspaces offered by organometallic polymers. The challenges that remain and the need for additional methodological developments necessary to further strengthen the co-design concept are then presented.

Herein, the fabrication of all-organic conductive wires is demonstrated by utilizing patterning techniques such as inkjet printing and sponge stencil to apply poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT:PSS) onto nonwoven polyethylene terephthalate (PET) fabric. The coating of the conducting polymer is only present on the surface of the substrate (penetration depth ∼ 200 μm) to retain the functionality and wearability of the textile. The wires fabricated by different patterning techniques provide a wide range of resistance, i.e., tens of kΩ/□ to less than 2 Ω/□ that allows the resistance to be tailored to a specific application. The sheet resistance is measured to be as low as 1.6 Ω/□, and the breakdown current is as high as 0.37 A for a 1 mm wide line. The specific breakdown current exceeds the previously reported values of macroscopic carbon nanotube based materials. Simple circuits composed of the printed wires are demonstrated, and resistance of the circuit from the measurement agrees with the calculated value based on Kirchhoff's rules. Additionally, the printed PEDOT:PSS wires show less than 6.2% change in sheet resistance after three washing and drying cycles using detergent.

Electrocardiography (ECG) is an essential technique for analyzing and monitoring cardiovascular physiological conditions such as arrhythmia. This article demonstrates the integration of screen-printed ECG circuitry from a commercially available conducting polymer, PEDOT:PSS, onto commercially available finished textiles. ECG signals were recorded in dry skin conditions due to the ability of PEDOT:PSS to function as both ionic and electronic conductors. The signal amplifies when the skin transpires water vapor or by applying a common lotion on the skin. Finally, PEDOT:PSS wires connected to PEDOT:PSS electrodes have been shown to record ECG signals comparable to Ag/AgCl connected to copper wires.

The dielectric constant of polymers was increased by combining flexible segments and rigid polar segments in the polymer backbone.

An all-organic fabric patch antenna is realized with the help of nanotemplates-assisted PEDOT:PSS conductive phase segregation, paving a new way for clothing integrated wearable electronic networks.

Recently, there has been a growing interest in developing wide band gap dielectric materials as the next generation insulators for capacitors, photovoltaic devices, and transistors. Organotin polyesters have shown promise as high dielectric constant, low loss, and high band gap materials. Guided by first-principles calculations from density functional theory (DFT), in line with the emerging codesign concept, the polymer poly(dimethyltin 3,3-dimethylglutarate), p(DMTDMG), was identified as a promising candidate for dielectric applications. Blends and copolymers of poly(dimethyltin suberate), p(DMTSub), and p(DMTDMG) were compared using increasing amounts of p(DMTSub) from 10% to 50% to find a balance between electronic properties and film morphology. DFT calculations were used to gain further insight into the structural and electronic differences between p(DMTSub) and p(DMTDMG). Both blend and copolymer systems showed improved results over the homopolymers with the films having dielectric constants of 6.8 and 6.7 at 10 kHz with losses of 1% and 2% for the blend and copolymer systems, respectively. The energy density of the film measured as a D-E hysteresis loop was 6 J/cc for the copolymer, showing an improvement compared to 4 J/cc for the blend. This improvement is hypothesized to come from a more uniform distribution of diacid repeat units in the copolymer compared to the blend, leading toward improved film quality and subsequently higher energy density.

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Flexible films having high dielectric constants with low dielectric loss have promising application in the emerging area of high‐energy‐density materials. Here, for the first time, an organometallic, Sn‐polyester‐containing hybrid free‐standing film in polyimide matrix is reported. Polyimide, pBTDA‐HDA, is used with poly(dimethyltin glutarate) and poly(dimethyltin‐3,3‐dimethyglutarate) (pDMTDMG) for having a processable film with tunable dielectric properties. Hybrid film with 60% pDMTDMG and 40% PI (HB2) is found to have improved dielectric features over previously synthesized organic polyimide and organometallic Sn‐polyester homopolymers. These novel organometallic–organic hybrid systems expanded a new area of dielectrics for next‐generation electronics with superior overall electrical performance.