Percolation by Brush Architecture: A Pathway toward Soft Electronics

Achieving simultaneous tissue-mimetic mechanical properties and electrical conductivity within a single molecular system remains a major challenge. Typically, the design of stretchable and flexible electronic materials requires a trade-off between mechanical compliance and electronic performance. Herein, we employ a computationally driven materials design strategy to synthesize polydimethylsiloxane bottlebrush graft copolymers with precisely controlled fractions of poly(3-hexylthiophene) (P3HT), where the grafts serve both as physical cross-links between bottlebrush strands and as conductive elements. Thin films cast from solution reveal percolation of P3HT needle-like crystals, corroborated by transmission electron microscopy, small-angle X-ray scattering, and computer simulations. These films exhibit a distinctive combination of properties, including a low elastic modulus (∼1-100 kPa) and an electrical conductivity of up to ∼10^-2 S/cm. Materials that simultaneously combine tissue-like mechanics with electronic functionality hold strong potential for wearable and implantable devices.