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Updated: Apr 17, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Dynamics of ground state absorption spectra in donor-acceptor pairs with ultrafast charge recombination
Roman G Fedunov1, Anastasiia V Plotnikova, Vladimir N Ionkin
1Volgograd State University , University Avenue 100, Volgograd 400062, Russia.
Abstract:
A theoretical approach to simulation of the transient spectra in molecular systems with ultrafast photoinduced nonradiative electronic transitions is developed. The evolution of the excited and ground state populations as well as the nonradiative transitions between them are calculated in the framework of the stochastic multichannel point-transition model involving the reorganization of the medium and the intramolecular high frequency vibrational modes. Simulations of transient spectra of donor-acceptor pairs excited in the charge-transfer band that are accompanied by ultrafast charge recombination into the ground state demonstrate a possibility of positive band appearance in the transient absorption spectrum caused by those systems in the ground state, which returned there from the excited state. The region of the parameters of the donor-acceptor systems where a positive ground state absorption signal can be observed is discussed. A qualitative comparison of the simulated transient spectra with the experimental data on betaine-30 is presented.
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