Enhancing Long-Range Energy Transport in Supramolecular Architectures by Tailoring Coherence Properties

Bernd Wittmann, Felix A. Wenzel, Stephan Wiesneth, Andreas T. Haedler, Markus Drechsler, Klaus Kreger, Jürgen Köhler, E. W. Meijer, Hans Werner Schmidt (Corresponding author), Richard Hildner (Corresponding author)

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Abstract

Efficient long-range energy transport along supramolecular architectures of functional organic molecules is a key step in nature for converting sunlight into a useful form of energy. Understanding and manipulating these transport processes on a molecular and supramolecular scale is a long-standing goal. However, the realization of a well-defined system that allows for tuning morphology and electronic properties as well as for resolution of transport in space and time is challenging. Here we show how the excited-state energy landscape and thus the coherence characteristics of electronic excitations can be modified by the hierarchical level of H-type supramolecular architectures. We visualize, at room temperature, long-range incoherent transport of delocalized singlet excitons on pico- to nanosecond time scales in single supramolecular nanofibers and bundles of nanofibers. Increasing the degree of coherence, i.e., exciton delocalization, via supramolecular architectures enhances exciton diffusivities up to 1 order of magnitude. In particular, we find that single supramolecular nanofibers exhibit the highest diffusivities reported for H-aggregates so far.

Original languageEnglish
Pages (from-to)8323-8330
Number of pages8
JournalJournal of the American Chemical Society
Volume142
Issue number18
DOIs
Publication statusPublished - 6 May 2020

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    Wittmann, B., Wenzel, F. A., Wiesneth, S., Haedler, A. T., Drechsler, M., Kreger, K., Köhler, J., Meijer, E. W., Schmidt, H. W., & Hildner, R. (2020). Enhancing Long-Range Energy Transport in Supramolecular Architectures by Tailoring Coherence Properties. Journal of the American Chemical Society, 142(18), 8323-8330. https://doi.org/10.1021/jacs.0c01392