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FUBSSY Report Summary

Project ID: 267563
Funded under: FP7-IDEAS-ERC
Country: Switzerland

Final Report Summary - FUBSSY (Functional Biosupramolecular Systems: Photosystems and Sensors)

The general objective of this proposal was “to secure access to supramolecular functional systems for use in materials, chemical and biological sciences.” Arguably most important among the specific objectives was the development synthetic methods to build functional surface architectures of highest possible sophistication with highest possible precision. This is important because in nature, most significant function is achieved by most complex molecular architectures, and no one really knows what we would get if we would be able to build organic materials of similar complexity with similar precision. To help improving on this situation, four general synthetic methods to build multicomponent architectures directly on solid surfaces have been invented during this grant period (now increasingly referred to as SOSIP, TSE, TSS and TDC). These methods could only be realized with new, often non-conventional concepts (such as, for the expert: orthogonal dynamic covalent bonds, surface-initiated ring-opening disulfide-exchange polymerization, stack exchange, self-sorting, self-repair). Once established, they have been used to ask important questions concerning organic photosystems that previously could not be asked because the required structures simply could not be made. Most intriguing was the construction of double-channel photosystems with antiparallel redox gradients composed of up to three components each. Arguably the most sophisticated functional surface architecture realized so far, triple-gradient double-channel photosystems successfully transcribe one of the most advanced lesson from nature toward the materials sciences. Namely, with antiparallel gradients in co-axial channels to drive holes and electrons apart right after their generation with light, the loss of photonic energy by charge recombination dropped from 29% to 2%. Other topics besides these “OMARG-SHJs” that became accessible with the new synthetic methods include triple-channel, ion-gated and dipolar photosystems.

Over the past five years, the integration of unorthodox interactions proved decisive to create a rich collection of functional systems that reaches far beyond multicomponent photosystems on solid surfaces. Realized examples include the use of hydrazone exchange to build an artificial nose, disulfide exchange to find completely new ways to enter into cells, mechanosensitive bonds for conceptually innovative fluorescent membrane probes, or halogen bonds to transport anions across lipid bilayer membranes. Moreover, ionpair-pi interactions have been introduced and applied to spectral tuning and the activation of cell-penetrating peptides. Most important certainly is the discovery of anion-pi catalysis, that is the use of anion-pi interactions to realize chemical transformations on aromatic surfaces. This is a totally new fundamental concept in chemistry. Overall, this focus on unorthodox interactions at work has allowed us to tackle several important longstanding challenges from a new angle, the results have game-changing potential and provide most attractive perspectives for the continuation.

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