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

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Department of Chemistry and Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
§ Department of Chemistry and Biochemistry, Center for Discovery and Innovation, The City College of New York of The City University of New York, 160 Convent Avenue, New York, New York 10031 United States
Cite this: Nano Lett. 2016, 16, 11, 6808–6815
Publication Date (Web):September 30, 2016
Copyright © 2016 American Chemical Society

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    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.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.nanolett.6b02529.

    • Additional details on modeling, simulating, and measuring exciton annihilation. Figures showing typical absorption and emission spectra from all temperatures, full width half max for four sets of temperature-dependent experiments, inner and outer wall peak ratios follow a Boltzmann distribution, lifetime and quantum yield increases, the experimental setup for studying EEA, a plot of PL intensity under continuous excitation at 530 nm, an estimate of the number of aggregates that can participate in EEA as a function of excitation density and length of aggregate, a plot of the stick spectrum of the dipole weighted eigenvalues of a single aggregate Hamiltonian with 600 cm–1 of diagonal disorder, and a plot of exciton wavefunction. Tables showing fit parameters obtained with the model in eq S9 for the absorption and emission spectra and from eq S11 in different temperature-dependent experiments. (PDF)

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