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Abstract Stretchable polymer semiconductors (PSCs) have seen great advancements alongside the development of soft electronics. But it remains a challenge to simultaneously achieve high charge carrier mobility and stretchability. Herein, we report the finding that stretchable PSC thin films (<100-nm-thick) with high stretchability tend to exhibit multi-modal energy dissipation mechanisms and have a large relative stretchability ( rS ) defined by the ratio of the entropic energy dissipation to the enthalpic energy dissipation under strain. They effectively recovered the original molecular ordering, as well as electrical performance, after strain was released. The highest rS value with a model polymer (P4)more » exhibited an average charge carrier mobility of 0.2 cm ² V ⁻¹ s ⁻¹ under 100% biaxial strain, while PSCs with low rS values showed irreversible morphology changes and rapid degradation of electrical performance under strain. These results suggest rS can be used as a parameter to compare the reliability and reversibility of stretchable PSC thin films.« less

Polymer semiconductors (PSCs) are a desirable class of materials for next-generation electronics. However, the conformational complexity associated with macromolecules, as well as the presence of unique inter- and intrachain interactions, make it challenging to control the morphology of PSCs. Previously, it has been reported that beyond a certain molecular weight, thin-film charge carrier mobility typically drops due to reduced crystallinity and increased entanglement. In this work, the use of an insulating secondary matrix polymer, polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene (SEBS), is shown to induce molecular ordering of PSCs across multiple length scales. Aggregation-induced molecular ordering in SEBS/PSC hybrid films is strongly correlated to themore » molecular weight of the semiconducting component. The higher the molecular weight of PSC used to blend with SEBS, the greater the observed improvement in polymer aggregation and orientation. This leads to a 5-fold increase of charge carrier mobility, from 0.3 to 1.5 cm2 V^–1 s^–1 (P-97k), in field-effect transistors (FETs) with only 30 wt % of the semiconducting polymer in SEBS. Moreover, mobility can be further elevated to 2 cm2 V^–1 s^–1 using an extensional flow-driven solution shearing deposition method. The findings here on using a secondary polymer matrix to dramatically improve the molecular organization and charge transport of a high-molecular-weight PSC are a useful morphological control strategy. It can also be carried out using nonhalogenated solvents, such as $$p$$-xylene, which are more environmentally benign and industrially relevant than commonly used chlorinated solvents.« less

Deformable electronic devices that are impervious to mechanical influence when mounted on surfaces of dynamically changing soft matters have great potential for next–generation implantable bioelectronic devices. Here, deformable field–effect transistors (FETs) composed of single organic nanowires (NWs) as the semiconductor are presented. The NWs are composed of fused thiophene diketopyrrolopyrrole based polymer semiconductor and high–molecular–weight polyethylene oxide as both the molecular binder and deformability enhancer. The obtained transistors show high field–effect mobility >8 cm² V^–1 s^–1 with poly(vinylidenefluoride–co–trifluoroethylene) polymer dielectric and can easily be deformed by applied strains (both 100% tensile and compressive strains). The electrical reliability and mechanical durabilitymore » of the NWs can be significantly enhanced by forming serpentine–like structures of the NWs. Remarkably, the fully deformable NW FETs withstand 3D volume changes (>1700% and reverting back to original state) of a rubber balloon with constant current output, on the surface of which it is attached. In conclusion, the deformable transistors can robustly operate without noticeable degradation on a mechanically dynamic soft matter surface, e.g., a pulsating balloon (pulse rate: 40 min^–1 (0.67 Hz) and 40% volume expansion) that mimics a beating heart, which underscores its potential for future biomedical applications.« less

The design of polymer semiconductors possessing high charge transport performance, coupled with good ductility, remains a challenge. Understanding the distribution and behavior of both crystalline domains and amorphous regions in conjugated polymer films, upon an applied stress, shall provide general guiding principles to design stretchable organic semiconductors. Structure–property relationships (especially in both side chain and backbone engineering) are investigated for a series of poly(tetrathienoacene-diketopyrrolopyrrole) polymers. It is observed that the fused thiophene diketopyrrolopyrrole-based polymer, when incorporated with branched side chains and an additional thiophene spacer in the backbone, exhibits improved mechanical endurance and, in addition, does not show crack propagationmore » until 40% strain. Furthermore, this polymer exhibits a hole mobility of 0.1 cm2 V^-1 s^-1 even at 100% strain or after recovered from strain, which reveals prominent continuity and viscoelasticity of the polymer thin film. In conclusion, it is also observed that the molecular packing orientations (either edge-on or face-on) significantly affect the mechanical compliance of the polymer films. The improved stretchability of the polymers is attributed to both the presence of soft amorphous regions and the intrinsic packing arrangement of its crystalline domains.« less