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

Titelangaben

Wittmann, Bernd ; Wenzel, Felix A. ; Wiesneth, Stephan ; Haedler, Andreas T. ; Drechsler, Markus ; Kreger, Klaus ; Köhler, Jürgen ; Meijer, E. W. ; Schmidt, Hans-Werner ; Hildner, Richard:
Enhancing Long-Range Energy Transport in Supramolecular Architectures by Tailoring Coherence Properties.
In: Journal of the American Chemical Society. Bd. 142 (2020) Heft 18 . - S. 8323-8330.
ISSN 1520-5126
DOI der Verlagsversion: https://doi.org/10.1021/jacs.0c01392

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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.