Investigating the Mobility-Compressibility Properties of Conjugated Polymers by the Contact Film Transfer Method with Prestrain.

Up to now, researches on the mobility-stretchability of semiconducting polymers are extensively investigated, but little attention was  paid to their morphology and field-effect transistor characteristics under compressive strains, which is equally crucial in wearable electronic applications. In this work, a contact film transfer method is applied to evaluate the mobility-compressibility properties of conjugated polymers. A series of isoindigo-bithiophene conjugated polymers with symmetric carbosilane side chains (P(SiSi)), siloxane-terminated alkyl side chains (P(SiOSiO)), and combined asymmetric side chains (P(SiOSi)) are investigated. Accordingly, a compressed elastomer slab is used to transfer and compress the polymer films by releasing prestrain, and the morphology and mobility evolutions of these polymers are tracked. It is found that P(SiOSi) outperforms the other symmetric polymers including P(Si─Si) and P(SiO─SiO), having the ability to dissipate strain with its shortened lamellar spacing and orthogonal chain alignment. Notably, the mechanical durability of P(SiOSi) is also enhanced after consecutive compress-release cycles. In addition, the contact film transfer technique is demonstrated to be applicable to investigate the compressibility of different semiconducting polymers. These results demonstrate a comprehensive approach to understand the mobility-compressibility properties of semiconducting polymers under tensile and compressive strains.

Unraveling the Effect of Stereoisomerism on Mobility-Stretchability Properties of n-Type Semiconducting Polymers with Biobased Epimers as Conjugation Break Spacers.

The development of intrinsically stretchable n-type semiconducting polymers has garnered much interest in recent years. In this study, three biobased dianhydrohexitol epimers of isosorbide (ISB), isomannide (IMN), and isoidide (IID), derived from cellulose, were incorporated into the backbone of a naphthalenediimide (NDI)-based n-type semiconducting polymer as conjugation break spacers (CBSs). Accordingly, three polymers were synthesized through the Migita-Kosugi-Stille coupling polymerization with NDI, bithiophene, and CBSs, and the mobility-stretchability properties of these polymers were investigated and compared with those of their analogues with conventional alkyl-based CBSs. Experimental results showed that the different configurations of these epimers in CBSs sufficiently modulate the melt entropies, surface aggregation, crystallographic parameters, chain entanglements, and mobility-stretchability properties. Comparable ductility and edge-on preferred stacking were observed in polymers with endo- or exo-configurations in IMN- and IID-based polymers. By contrast, ISB with endo-/exo-configurations exhibits an excellent chain-realigning capability, a reduced crack density, and a proceeding bimodal orientation under tensile strain. Therefore, the ISB-based polymer exhibits high orthogonal electron mobility retention of (53 and 56)% at 100% strain. This study is one of the few examples where biobased moieties are incorporated into semiconducting polymers as stress-relaxation units. Additionally, this is the first study to report on the effect of stereoisomerism of epimers on the morphology and mobility-stretchability properties of semiconducting polymers.