Supramolecular chemistry has long been interested in the self-assembly state of molecules and its influence on their tangible properties. The ability to control the self-assembled state opens up opportunities to design materials with specific properties such as charge transport capability and fluorescence wavelength. Scientists have been delving into the impact of molecular organization on the properties of supramolecular assemblies at the nano and mesoscopic scales. However, the dynamic structural changes and lack of control over self-assemblies often pose challenges in studying such structures.

A recent study published in the Journal of the American Chemical Society focused on investigating the properties of one-dimensional mesoscale supramolecular assemblies composed of the same luminescent molecule but with two different structures. The study, led by Prof. Shiki Yagai from Chiba University, unveiled how the properties of these structures varied depending on whether the molecules were arranged in a closed circular pattern or not. The research involved a team of experts from Chiba University, Tokyo Institute of Technology, and Osaka University.

Prof. Yagai emphasized the geometrical beauty of circular structures, highlighting the allure of structures without termini or corners. The synthesis of giant cyclic molecules to create beautiful structures has been a pursuit in chemistry, aiming to achieve elegance in the synthesis process. Nature itself showcases the functional beauty of circular structures, as seen in the light-harvesting antenna organ of purple photosynthetic bacteria, where arranging chlorophyll dyes in a circular array enhances light collection and energy transfer.

Through the self-assembly of luminescent molecules, the research team obtained a mixture of terminus-free cyclic structures (toroids) and randomly coiled structures. The separation of these structures revealed that the closed toroidal structure exhibited higher energy and more efficient luminescence compared to random coils. Ultrafast laser spectroscopy was conducted to delve into the mechanism behind these topology-dependent fluorescence properties. The results indicated that random coils with termini lost excitation energy due to defects, while toroids maintained fluorescence without energy loss.

The study’s findings suggest that morphological control of materials at the mesoscale could serve as a new guideline for designing functional materials. The separation of different structures is crucial for analyzing their photophysical properties accurately, as energy transfer between structures can lead to biased results. The researchers believe that these insights could pave the way for the development of high-performance flexible devices utilizing cyclic molecular assemblies.

Prof. Yagai expressed optimism about the correlation between structural beauty and functional properties in meso-scale molecular assemblies. The potential to improve the performance of solar cell devices and light-emitting devices through these insights could lead to broader acceptance and enrichment of people’s lives. The study opens up new possibilities for leveraging structural beauty to enhance the functional capabilities of materials in various applications.


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