All-DFTB Approach to the Parametrization of the System-Bath Hamiltonian Describing Exciton-Vibrational Dynamics of Molecular Assemblies - Archive ouverte HAL Access content directly
Journal Articles Journal of Chemical Theory and Computation Year : 2018

All-DFTB Approach to the Parametrization of the System-Bath Hamiltonian Describing Exciton-Vibrational Dynamics of Molecular Assemblies

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Abstract

Spectral density functions are central to the simulation of complex many body systems. Their determination requires making approximations not only to the dynamics but also to the underlying electronic structure theory. Here, blending different methods bears the danger of an inconsistent description. To solve this issue we propose an all-DFTB approach to determine spectral densities for the description of Frenkel excitons in molecular assemblies. The protocol is illustrated for a model of a PTCDI crystal, which involves the calculation of monomeric excitation energies and Coulomb couplings between monomer transitions, as well as their spectral distributions due to thermal fluctuations of the nuclei. Using dynamically defined normal modes, a mapping onto the standard harmonic oscillator spectral densities is achieved.

Dates and versions

hal-02290267 , version 1 (17-09-2019)

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P. A. Plotz, J. Megow, Thomas Niehaus, O. Kuhn. All-DFTB Approach to the Parametrization of the System-Bath Hamiltonian Describing Exciton-Vibrational Dynamics of Molecular Assemblies. Journal of Chemical Theory and Computation, 2018, 14 (10), pp.5001-5010. ⟨10.1021/acs.jctc.8b00493⟩. ⟨hal-02290267⟩
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