Periodic Reporting for period 1 - SolSupPol (Understanding and exploiting competitive solvent interactions in supramolecular polymerization: from solutions to bulk materials)
Período documentado: 2021-08-01 hasta 2023-07-31
In the second part of the project, we exploited the self-assembly of functional monomers and the targeted tuning of the experimental conditions to implement and regulate singlet fission within supramolecular polymers. In the investigated systems, the H-bond driven assembly of a supramolecular scaffold guides the organization of the functional pendants into exohelical frameworks. Through-space interactions mediate fast singlet conversion, affording independent triplets with lifetimes exceeding those found in crystalline materials. Subtle changes in monomer design enable the modulation of excited state kinetics as a result of distinct molecular arrangements within the assemblies.
A detailed dissemination plan at different audience levels guaranteed the high impact of this research, strongly promoting further scientific advances in the research field and boosting applications.
On the other hand, the exploitation of one-dimensional supramolecular templates to enable SF within ordered nanostructures of photoactive pendants is unprecedent in literature. Leveraging directional secondary interactions between monomeric units provides a novel strategy to mitigate the strength of interchromophoric interactions, while imparting a supramolecular order reminiscent of crystalline materials. The results provides new insights in the quest for fast singlet conversion and long-lived triplets, highlighting the critical role of conformational dynamic and chiral organization in regulating excited-state dynamics within non-covalent, ordered architecture and outlining the potential of singlet fission to disclose the structure and dynamics of supramolecular polymers. The innovative implementation of singlet fission in supramolecular polymers contributes to elucidate the structure-property relationships regulating the process, addressing some of the major issues that currently limit the efficiency of singlet fission-based photovoltaics.
Overall, the work carried out within this project contributes towards addressing the global challenges of sustainability and clean energy of the United Nations and the European Green Deal. The outcomes of this high-gain research strongly contribute to advancements within the research field of supramolecular polymers, enabling the design of functional, adaptive materials based on supramolecular interactions and ultimately contributing to the knowledge-based society. On one hand, the knowledge gained from the study of solvent-induced circularly polarized emission will foster advances in a wide range of chirality-related applications. On the other hand, fundamental investigation on singlet fission is of crucial importance for applications in solar energy conversion schemes.