Excitonic interactions and stark spectroscopy of light harvesting systems

Article Abstract:

A new Green function expression for the Stark signal of molecular aggregates from the third-order nonlinear response to the total field has been derived. The new formulation does not suffer from singularities when the exciton states are nearly degenerate and avoids the computation of two-exciton states. The Stark spectrum is expressed as the sum of Type I and II contributions. The former has the shape of the first and second derivative of the line shape function. The latter depend on transitions within the one-exciton band.

Analysis, Exciton theory, Excitons, Excited state chemistry

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Superradiance coherence sizes in single-molecule spectroscopy of LH2 antenna complexes

Article Abstract:

A study was conducted to analyze the distribution of radiative lifetimes resulting from a static disorder mechanism for exciton localization. The distributions of radiative decay rates in circular aggregates for two extreme dipole orientations of chromophores were examined. Results provide detailed characterizations of the electronic state properties. Findings also showed that the lower-energy excitations are the exciton type with delocalization over the entire aggregate.

Electronic structure, Atomic structure

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Superradiance of aggregated thiacarbocyanine molecules

Article Abstract:

Steady-state fluorescence and time-resolve fluorescence lifetime measurements have been undertaken for 3,3'-diethyl-5,5'-dichloro-9-phenylthiacarbocyanine in methanol and in aqueous homogenous solution. Superradiance plays a vital role in optical dynamics of the aggregated system.

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