Periodic Reporting for period 4 - LifeLikeMat (Dissipative self-assembly in synthetic systems: Towards life-like materials)
Reporting period: 2023-08-01 to 2024-12-31
We drew inspiration from living organisms as sophisticated self-assembled structures that exist and operate far from thermodynamic equilibrium to develop new principles for designing synthetic dissipative self-assembly systems and to fabricate new dynamic supramolecular systems materials based on these principles. Consequently, this research led to light-sensitive nanoparticle assemblies, ATP-driven colloidal crystals, supramolecular machinery for disequilibrating azobenzenes, among other dynamic materials and systems. In the long run, the results obtained in the course of this project could impact a range of industries, including the pharmaceutical and energy sectors.
The main results obtained from the beginning of the project include the development of novel nanostructured materials by electrostatic coassembly of oppositely charged nanoparticles and small molecules, encapsulation-induced improvement of fatigue resistance of a molecular photoswitch, a novel tool of modulation of the optical properties of fluorescent dyes via noncovalent dimerization, development of photosensitive adhesives for colloidal particles, demonstration of azobenzene and spiropyran switching in the solid state by adsorption within nanoporous networks, dissipative self-assembly of nanoparticles chemically fueled by ATP, morphology control in crystalline nanoparticle–polymer aggregates, design and synthesis of adaptive supramolecular hosts capable of guest-induced symmetry change, development of a supramolecular tool for activating azobenzenes with red light, and the discovery of new crystalline phases in binary nanoparticle superlattices. Overall, the results of this project have been disseminated at multiple conferences and symposia worldwide (two of which the PI co-organized: the Gordon Research Conference Self-Assembly and Supramolecular Chemistry and the Gordon Research Conference Systems Chemistry) and published in 16 papers so far (cited >900 times to date), with several others under review and/or prepared for submission.
These research efforts resulted in a diverse portfolio of dissipative supramolecular systems and materials, ranging from light-sensitive nanoparticle assemblies and ATP-driven colloidal crystals to supramolecular machinery for disequilibrating azobenzenes. We also developed conceptually new tools for the characterization of dissipative self-assembly processes, such as monitoring light emission from ternary host-guest complexes. The results of the project go significantly beyond the state-of-the-art, as evidenced by publications in recognized journals (including Chem, Journal of the Americal Chemical Society, Science, and Nature Chemistry, with additional papers currently under review or prepared for publication).