Molecular-Scale\nGeometric Design: Zigzag-Structured\nIntrinsically Stretchable Polymer Semiconductors

Orienting\nintelligence and multifunction, stretchable semiconductors\nare of great significance in constructing next-generation human-friendly\nwearable electronic devices. Nevertheless, rendering semiconducting\npolymers mechanical stretchability without compromising intrinsic\nelectrical performance remains a major challenge. Combining geometry-innovated\ninorganic systems and structure-tailored organic semiconductors, a\nmolecular-scale geometric design strategy is proposed to obtain high-performance\nintrinsically stretchable polymer semiconductors. Originating from\nthe linear regioregular conjugated polymer and corresponding <i>para</i>-modified near-linear counterpart, a series of zigzag-structured\nsemiconducting polymers are developed with diverse <i>ortho</i>-type and <i>meta</i>-type kinking units quantitatively\nincorporated. They showcase huge edges in realizing stretchability\nenhancement for conformational transition, likewise with long-range\nπ-aggregation and short-range torsion disorder taking effect.\nAssisted by additional heteroatom embedment and flexible alkyl-chain\nattachment, mechanical stretchability and carrier mobility could afford\na two-way promotion. Among zigzag-structured species, <i>o</i>-OC8–5% with the initial field-effect mobility up to 1.92\ncm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup> still delivers\n1.43 and 1.37 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup> under 100% strain with charge transport parallel and perpendicular\nto the stretching direction, respectively, accompanied by outstanding\nperformance retention and cyclic stability. This molecular design\nstrategy contributes to an in-depth exploration of prospective intrinsically\nstretchable semiconductors for cutting-edge electronic devices.