Exciton Coherence Lifetimes from Electronic Structure

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Exciton Coherence Lifetimes from Electronic Structure

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Title: Exciton Coherence Lifetimes from Electronic Structure
Author: Parkhill, John Anthony; Aspuru-Guzik, Alan; Tempel, David Gabriel

Note: Order does not necessarily reflect citation order of authors.

Citation: Parkhill, John A., David G. Tempel, and Alan Aspuru-Guzik. 2012. Exciton coherence lifetimes from electronic structure. Journal of Chemical Physics 136(10): 104510.
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Abstract: We model the coherent energy transfer of an electronic excitation within covalently linked aromatic homodimers from first-principles. Our results shed light on whether commonly used models of the bath calculated via detailed electronic structure calculations can reproduce the key dynamics. For the systems we model, the time scales of coherent transport are experimentally known from time-dependent polarization anisotropy measurements, and so we can directly assess whether current techniques are predictive for modeling coherent transport. The coupling of the electronic degrees of freedom to the nuclear degrees of freedom is calculated from first-principles rather than assumed, and the fluorescence anisotropy decay is directly reproduced. Surprisingly, we find that although time-dependent density functional theory absolute energies are routinely in error by orders of magnitude more than the coupling energy between monomers, the coherent transport properties of these dimers can be semi-quantitatively reproduced from these calculations. Future directions which must be pursued to yield predictive and reliable models of coherent transport are suggested.
Published Version: doi:10.1063/1.3689858
Terms of Use: This article is made available under the terms and conditions applicable to Other Posted Material, as set forth at http://nrs.harvard.edu/urn-3:HUL.InstRepos:dash.current.terms-of-use#LAA
Citable link to this page: http://nrs.harvard.edu/urn-3:HUL.InstRepos:8514994
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