Towards dual light control of a catalytically-driven chemical reaction cycle

Abstract

Chemically-fueled chemical reaction networks (CRNs) are key in controlling dissipative self-assembly. Having catalysts gating fuel consumption for both the activation and deactivation chemistry of (assembly-prone) monomers and controlling the catalytic activity with an external stimulus would provide better control over where, when, and how long self-assembled structures can form. Here we achieve light control over monomer activation and subsequent assembly into supramolecular fibers, and partial light control over deactivation and fiber disassembly. Activation proceeds via photoredox catalysis under visible light, whereas deactivation is achieved by organometallic catalysis that relies on a photocaged pre-fuel activated by ultraviolet light. Overall, we show how supramolecular fibers can be formed by visible light and how their destruction is accelerated by ultraviolet light.