Stretchable semiconducting polymers have been developed as a key component to enable skin-like wearable electronics, but their electrical performance must be improved to enable more advanced functionalities. Here, we report a solution processing approach that can achieve multi-scale ordering and alignment of conjugated polymers in stretchable semiconductors to substantially improve their charge carrier mobility. Using solution shearing with a patterned microtrench coating blade, macroscale alignment of conjugated-polymer nanostructures was achieved along the charge transport direction. In conjunction, the nanoscale spatial confinement aligns chain conformation and promotes short-range π-π ordering, substantially reducing the energetic barrier for charge carrier transport. As a result, the mobilities of stretchable conjugated-polymer films have been enhanced up to threefold and maintained under a strain up to 100%. This method may also serve as the basis for large-area manufacturing of stretchable semiconducting films, as demonstrated by the roll-to-roll coating of metre-scale films.

/pdf/multi-scale-ordering-in-highly-stretchable-polymer-20e1qm1i36.pdf

Multi-scale ordering in highly stretchable polymer semiconducting films.

Polymer semiconductors have been experiencing a remarkable improvement in electronic and optoelectronic properties, which are largely related to the recent development of a vast library of high-performance, donor-acceptor copolymers showing alternation of chemical moieties with different electronic affinities along their backbones. Such steady improvement is making conjugated polymers even more appealing for large-area and flexible electronic applications, from distributed and portable electronics to healthcare devices, where cost-effective manufacturing, light weight, and ease of integration represent key benefits. Recently, a strong boost to charge carrier mobility in polymer-based field-effect transistors, consistently achieving the range from 1.0 to 10 cm2 V-1 s-1 for both holes and electrons, has been given by uniaxial backbone alignment of polymers in thin films, inducing strong transport anisotropy and favoring enhanced transport properties along the alignment direction. Herein, an overview on this topic is provided with a focus on the processing-structure-property relationships that enable the controlled and uniform alignment of polymer films over large areas with scalable processes. The key aspects are specific molecular structures, such as planarized backbones with a reduced degree of conformational disorder, solution formulation with controlled aggregation, and deposition techniques inducing suitable directional flow.

Uniaxial Alignment of Conjugated Polymer Films for High‐Performance Organic Field‐Effect Transistors

The exciton-polaritons formed using carbon nanotube field-effect transistors strongly coupled to an optical microcavity can sustain electrical pumping under high current densities.

/pdf/electrical-pumping-and-tuning-of-exciton-polaritons-in-3juejc0tpb.pdf

Electrical pumping and tuning of exciton-polaritons in carbon nanotube microcavities.

Recent demonstrations of inverted thermal activation of charge mobility in polymer field-effect transistors have excited the interest in transport regimes not limited by thermal barriers. However, rationalization of the limiting factors to access such regimes is still lacking. An improved understanding in this area is critical for development of new materials, establishing processing guidelines, and broadening of the range of applications. Here we show that precise processing of a diketopyrrolopyrrole-tetrafluorobenzene-based electron transporting copolymer results in single crystal-like and voltage-independent mobility with vanishing activation energy above 280 K. Key factors are uniaxial chain alignment and thermal annealing at temperatures within the melting endotherm of films. Experimental and computational evidences converge toward a picture of electrons being delocalized within crystalline domains of increased size. Residual energy barriers introduced by disordered regions are bypassed in the direction of molecular alignment by a more efficient interconnection of the ordered domains following the annealing process. Though solution-processed conjugated polymers with inverted temperature activated transport have been reported, the origin of this behaviour is unclear. Here, the authors realize temperature-independent electron transport above 280 K in a donor-acceptor copolymer through microstructural engineering.

/pdf/microstructural-control-suppresses-thermal-activation-of-3ivif57okj.pdf

Microstructural control suppresses thermal activation of electron transport at room temperature in polymer transistors

The improvement of the performance of organic thin-film transistors is driven by novel materials and improved device engineering. Key developments are a continuous increase of the charge carrier mobility, a scale-down of transistor dimensions, and the reduction of contact resistance. Furthermore, new transistor designs such as vertical devices are introduced to benefit from drastically reduced channel length while keeping the effort for structuring moderate. Here, we show that a strong electrothermal feedback occurs in organic transistors, ultimately leading to output characteristics with regions of S-shaped negative differential resistance. For that purpose, we use an organic permeable-base transistor (OPBT) with outstanding current densities, where a strong and reproducible, non-linear electrothermal feedback is revealed. We derive an analytical description of the temperature dependent current-voltage behavior and offer a rapid investigation method for material systems, where a temperature-activated conductivity can be observed.

Non-Linear Self-Heating in Organic Transistors Reaching High Power Densities.

The channel temperature (Tch) of solution-processed 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS pentacene) thin film transistors (TFTs) is closely monitored in real time during current–voltage (I–V) measurements carried out in a He exchange gas cryostat at various base temperatures (Tb) between 300 K and 20 K. This is done using a platinum (Pt) resistance temperature sensor embedded within the transistor channel. Under large gate (Vg) and source-drain (Vds) voltage biases, an increase in Tch is observed, the magnitude of which depends on the thermal conductivity of the substrate. The increase in Tch is associated with a simultaneous increase in the transistor drain current (Id) and becomes particularly pronounced at cryogenic Tb. These experimental observations are rationalized using a 1D theoretical model and are attributed to current-induced Joule heating. However, even though the heating of the channel unquestionably plays an important role, the corresponding amount of increase in Id at cryogenic Tb and large voltage biases cannot be fully accounted for unless at low temperatures μTIPS is enhanced in the presence of strong electrical fields. Therefore it is concluded that the I–V characteristics of TIPS pentacene TFTs at low Tb and large voltage biases are a result of a complex interplay between current-induced Joule heating and electrical field effects.

Current-Induced Joule Heating and Electrical Field Effects in Low Temperature Measurements on TIPS Pentacene Thin Film Transistors

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Current-Induced Joule Heating and Electrical Field Effects in Low Temperature Measurements on TIPS Pentacene Thin Film Transistors