Light-Driven Rheological Modulation of Solventless Polymer Networks Enabled by Precisely Architected Flexible Star Polysiloxanes

Abstract

We report the synthesis and photoresponsivity of precisely designed liquid star-shaped poly(dimethyl siloxane) (PDMS) with anthracene end groups. Owing to the efficient end-linking of the flexible PDMS arms upon the first UV irradiation (λ = 365 nm, UV365), the storage modulus (G’) increased from 4.7 Pa to 119 kPa (>25,000-fold), and the physical state became a rubbery solid. Subsequent irradiation with UV light at a shorter wavelength (λ = 254 nm, UV254) decreased G’ toward the photostationary state, and viscoelasticity modulation was achieved between the two photostationary states under solvent-free conditions.