Multiscale modeling of molecular structure and optical properties of complex supramolecular aggregates

Anna S. Bondarenko, Ilias Patmanidis, Riccardo Alessandri, Paulo C. T. Souza, Thomas L. C. Jansen, Alex H. de Vries, Siewert J. Marrink*, Jasper Knoester*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

18 Citations (Scopus)
104 Downloads (Pure)


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.

Original languageEnglish
Pages (from-to)11514-11524
Number of pages11
JournalChemical Science
Issue number42
Publication statusPublished - 14-Nov-2020


  • DYE
  • CCDC 2003150: Experimental Crystal Structure Determination

    Yot, P. G. (Contributor), Weiss, M. S. (Contributor), Ehrling, S. (Contributor), Wallacher, D. (Contributor), Llewellyn, P. L. (Contributor), Coudert, F. (Contributor), Evans, J. D. (Contributor), Bon, V. (Contributor), Krause, S. (Contributor), Senkovska, I. (Contributor), Kaskel, S. (Contributor), Iacomi, P. (Contributor), Zheng, B. (Contributor), Maurin, G. (Contributor) & Többens, D. M. (Contributor), University of Groningen, 1-Jan-2020


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