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Updated: Jul 1, 2025

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
General model of nonradiative excitation energy migration on a spherical nanoparticle with attached chromophores
L Kułak1, A Schlichtholz2, P Bojarski3
1Faculty of Applied Physics and Mathematics, Gdańsk University of Technology, 80-233, Gdańsk, Poland.
Abstract:
Theory of multistep excitation energy migration within the set of chemically identical chromophores distributed on the surface of a spherical nanoparticle is presented. The Green function solution to the master equation is expanded as a diagrammatic series. Topological reduction of the series leads to the expression for emission anisotropy decay. The solution obtained behaves very well over the whole time range and it remains accurate even for a high number of the attached chromophores. Emission anisotropy decay depends strongly not only on the number of fluorophores linked to the spherical nanoparticle but also on the ratio of critical radius to spherical nanoparticle radius, which may be crucial for optimal design of antenna-like fluorescent nanostructures. The results for mean squared excitation displacement are provided as well. Excellent quantitative agreement between the theoretical model and Monte-Carlo simulation results was found. The current model shows clear advantage over previously elaborated approach based on the Padé approximant.
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