Systems chemistry: new external stimuli, molecular tools and applications

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Research on artificial chemical systems is expected to help us better understand some of the complex system effects in cell biology, and to find practical applications in molecular sensing, parallel chemical computing and material science. Systems chemistry is a young discipline that looks closely at the long-ignored dynamic processes occurring in complex chemical mixtures. Of particular interest are molecular networks that exhibit the ‘far-from-equilibrium’ phenomena ubiquitously found in macroscopic and (sub-)microscopic biological systems: self-replication, sustained (chemical) oscillations or non-linear responses to stimuli. Open questions in this area include: how can out-of-equilibrium systems best be created and what are suitable energy sources? Which transformations comprise the toolbox of systems chemistry? What are possible applications?The proposed research program will address all of these challenges by exploring new physical stimuli for the perturbation of dynamic molecular networks, developing a largely overlooked reversible covalent reaction ideally suited for molecular sensing, and approaching the chemistry of synthetic carbon allotropes, for the first time, from a systems chemistry perspective.In subproject 1, ultrasound and pH-oscillators will be coupled with dynamic combinatorial libraries to produce out-of-equilibrium effects, such as self-sorting, chemical oscillations and directional translational motion in a sonication-driven molecular motor. In subproject 2, the acid-lability and tripodal structure of orthoesters will be exploited for the templated self-assembly of new dynamic macrocycles, as well as C3-symmetric cryptands, and the potential of such architectures for sensing of organic molecules and metal cations will be explored. In subproject 3, the reach of systems chemistry will be extended to three different types of fullerenes and graphene oxide, whose reversible covalent functionalization could open up opportunities for applications in organic electronic devices.