Multiscale modeling of molecular structure and optical properties of complex supramolecular aggregates. Issue 42 (6th October 2020)

• Record Type: Journal Article
• Authors: Bondarenko, Anna S.; Patmanidis, Ilias; Alessandri, Riccardo; Souza, Paulo C. T.; Jansen, Thomas L. C.; de Vries, Alex H.; Marrink, Siewert J.; Knoester, Jasper
• Is Part Of: Chemical science. Volume 11:Issue 42(2020)
• Page Start: 11514
• Page End: 11524
• Publication Date: 2020-10-06
• Subjects: Chemistry -- Periodicals; 540.5
• DOI: 10.1039/d0sc03110k
• Languages: English
• ISSNs: 2041-6520

Abstract

Abstract : Multiscale modeling resolves the molecular structure of a synthetic light-harvesting complex, unraveling the microscopic origin of its photophysical properties. Abstract : Supramolecular aggregates of synthetic dye molecules offer great perspectives to prepare biomimetic functional materials for light-harvesting and energy transport. The design is complicated by the fact that structure–property relationships are hard to establish, because the molecular packing results from a delicate balance of interactions and the excitonic properties that dictate the optics and excited state dynamics, in turn sensitively depend on this packing. Here we show how an iterative multiscale approach combining molecular dynamics and quantum mechanical exciton modeling can be used to obtain accurate insight into the packing of thousands of cyanine dye molecules in a complex double-walled tubular aggregate in close interaction with its solvent environment. Our approach allows us to answer open questions not only on the structure of these prototypical aggregates, but also about their molecular-scale structural and energetic heterogeneity, as well as on the microscopic origin of their photophysical properties. This opens the route to accurate predictions of energy transport and other functional properties.