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Exciton transport in dynamically disordered molecular aggregates: influence on optical line shapes

For Frenkel excitons moving on a linear trimer we investigate the influence of dynamic disorder on their optical line shapes. The dynamic disorder models the influence of vibrational degrees of freedom and is taken into account by fluctuations of the local excitation energy and of the transfer matri...

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Bibliographic Details
Published in:Chemical physics 1993-12, Vol.177 (3), p.715-726
Main Authors: Reineker, P., Warns, Ch, Neidlinger, Th, BarvĂ­k, I.
Format: Article
Language:English
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Summary:For Frenkel excitons moving on a linear trimer we investigate the influence of dynamic disorder on their optical line shapes. The dynamic disorder models the influence of vibrational degrees of freedom and is taken into account by fluctuations of the local excitation energy and of the transfer matrix element between neighbouring molecules. The fluctuations are represented by dichotomic Markov processes with coloured noise. We obtain a closed set of equations of motion for the correlation functions determining the optical line shape which is solved exactly as well as using various approximations. The line shapes are discussed for various sets of the model parameters. Furthermore we show that slower fluctuations need higher approximations in our factorization scheme. The limit of static fluctuations can only be covered by the full set of equations.
ISSN:0301-0104
DOI:10.1016/0301-0104(93)85034-6