Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate

We report 1.6 ± 1 μm exciton transport in self-assembled supramolecular light-harvesting nanotubes (LHNs) assembled from amphiphillic cyanine dyes. We stabilize LHNs in a sucrose glass matrix, greatly reducing light and oxidative damage and allowing the observation of exciton–exciton annihilation si...

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Bibliographic Details
Main Authors: Eisele, Dörthe M., Caram, Justin R, Doria, Sandra, Freyria, Francesca, Sinclair, Timothy Scott, Bawendi, Moungi G, Rebentrost, Frank, Lloyd, Seth
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:en_US
Published: American Chemical Society 2018
Online Access:http://hdl.handle.net/1721.1/113346
https://orcid.org/0000-0003-1192-4746
https://orcid.org/0000-0002-2710-5545
https://orcid.org/0000-0002-9371-6109
https://orcid.org/0000-0003-2220-4365
https://orcid.org/0000-0002-6728-8163
Description
Summary:We report 1.6 ± 1 μm exciton transport in self-assembled supramolecular light-harvesting nanotubes (LHNs) assembled from amphiphillic cyanine dyes. We stabilize LHNs in a sucrose glass matrix, greatly reducing light and oxidative damage and allowing the observation of exciton–exciton annihilation signatures under weak excitation flux. Fitting to a one-dimensional diffusion model, we find an average exciton diffusion constant of 55 ± 20 cm2/s, among the highest measured for an organic system. We develop a simple model that uses cryogenic measurements of static and dynamic energetic disorder to estimate a diffusion constant of 32 cm2/s, in agreement with experiment. We ascribe large exciton diffusion lengths to low static and dynamic energetic disorder in LHNs. We argue that matrix-stabilized LHNS represent an excellent model system to study coherent excitonic transport. Keywords: coherent exciton; exciton; exciton delocalization; exciton diffusion; J-aggregate; molecular aggregate