Publication date: 11th July 2022
The natural light-harvesting antennae of plants and photosynthetic bacteria are one of the most fascinating functional molecular nanoassemblies. Their unprecedented quantum efficiency relies on the strong coupling between thousands of densely packed chromophores giving rise to highly delocalized excitons which travels over long distances before reaching the reaction centre. However, the structural complexity of these systems leads to spectral congestion thereby blurring individual exciton transfer pathways that are vital to unravel for potential applications. Artificial model systems allow for better understanding of the structure-property relationship through reducing the complexity of natural light-harvesting complexes and disclosing the working principles to the basic elements.
Here we demonstrate a novel spectroscopic/microfluidics approach to deconvolute the supramolecular hierarchy and its connection to optical properties of a model system, multi-layered nanotubes [1-3]. They are based on the C8S3 molecules which self-assemble in an aqueous surrounding to a highly-ordered, concentric double-walled nanotubes (DWNTs) of 6/13 nm in inner/outer diameter and few micrometres in length. Each of these NTs can be considered as a quasi-2D molecular system (a plane wrapped into a tube) of strongly coupled molecules which results in highly delocalized and mobile excitonic states. We will presented a power platform of microfluidics, optical spectroscopy, and cryo-TEM, used to unravel the nature of exciton delocalization as well as exciton diffusion in DWNTs. We will also discuss the intermediate dynamical states of self-assembly via microfluidics manipulation of the structural hierarchy on the nanoscale via controlled alterations of individual sub-units of DWNT [4].
M.S.P and S.R.K. acknowledge financial support from the Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO, project OCENW.KLEIN.356)
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