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HJ-Aggregate Behavior of Crystalline 7,8,15,16-Tetraazaterrylene: Introducing a New Design Paradigm for Organic Materials

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    HJ-Aggregate Behavior of Crystalline 7,8,15,16-Tetraazaterrylene: Introducing a New Design Paradigm for Organic Materials
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    † Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United States
    ‡ ‡Department of Chemistry and §Department of Polymer Science and Engineering, University of Massachusetts, Amherst, Massachusetts 01002, United States
    ∥ Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2014, 118, 49, 28842–28854
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    https://doi.org/10.1021/jp509011u
    Published December 2, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    Absorption and photoluminescence properties of terrylene derivative 7,8,15,16-tetraazaterrylene (TAT) in its solution and crystal phases have revealed rather unusual spectral characteristics that defy classification in terms of simple H- or J-aggregate-coupled systems. TAT readily forms crystalline aggregates by either self-assembly in solution or physical vapor deposition, based on π stacks aligned roughly along the crystallographic a axis. Using a Holstein-style Hamiltonian including both Frenkel and charge-transfer (CT) excitons, the crystal absorption and steady-state photoluminescence (PL) spectra/line shapes are shown to be determined by a competition between long-range Coulombic coupling, which induces H-aggregate behavior, and short-range charge-transfer-mediated coupling, which induces J-like behavior. Such “HJ” aggregates display J-aggregate signatures in the low-energy region of the absorption spectrum and H-aggregate signatures at higher energies, which are in excellent agreement with our experiments. The H/J competition also results in a sharp reduction in the exciton bandwidth and the appearance of an exciton band minima at k ≈ ±π/2, where k is the dimensionless wave vector along the stacking axis. The presence of a band minimum for nonzero values of k bestows hybrid HJ behavior in the PL spectrum. We present a new design paradigm for organic electronic materials on the basis of the constructive or destructive interference of short- and long-range coupling, postulating the existence of HH, JJ, JH, and HJ aggregates with unique transport and radiative properties.

    Copyright © 2014 American Chemical Society

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    Supporting Information

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    Full Hamiltonian for a 3D TAT crystal, further information about the parametrization of the TAT molecules, the optimization of aggregate parameters, a comparison of B3LYP DFT- and PW91 DFT-calculated electron- and hole-transfer integrals, a description of how the PL spectrum is calculated, and an exploration of the absorption and PL spectra for other diabatic CT energies. This material is available free of charge via the Internet at http://pubs.acs.org.

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    This article is cited by 106 publications.

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    Cite this: J. Phys. Chem. C 2014, 118, 49, 28842–28854
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