4.6 Article

The fate of molecular excited states: modeling donor-acceptor dyes

期刊

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 24, 期 9, 页码 5555-5563

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cp05971h

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资金

  1. European Union [812872]
  2. COMP-HUB Initiative - Departments of Excellence program of the Italian Ministry for Education, University and Research (MIUR, 2018-2022)
  3. Alexander von Humboldt Foundation
  4. HPC (High Performance Computing) facility of the University of Parma, Italy

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In this study, we investigate the relaxation process of a coherently excited molecule using the Redfield approximation. The proposed molecular model successfully describes the fast vibrational relaxation and the slower relaxation towards the ground state. It is important to separately couple each vibration to an independent bath to avoid cross-talking between modes. The number of molecular vibrations introduced in the model does not affect the system dynamics, supporting the use of simplified models for donor-acceptor dyes with a single coupled vibration.
We investigate the relaxation of a coherently excited molecule in the Redfield approximation. The molecular model, parametrized to describe donor-acceptor dyes that represent a large family of molecules of interest for several applications, accounts for two diabatic electronic states non-adiabatically coupled to a few vibrational coordinates. The proposed approach successfully describes the fast vibrational relaxation, followed by a much slower relaxation towards the ground state, a physically relevant result that is robust vs. the specific model adopted for the system-bath coupling and the specific (reasonable) choice of the bath spectral density. We demonstrate that, when dealing with more than a single vibration, it is important that each vibration is separately coupled to an independent bath so as to avoid the cross-talking of the modes through their coupling to the same bath. Provided that the overall strength of the electron-vibration coupling is maintained constant, the number of molecular vibrations introduced in the model does not affect the system dynamics, supporting the use of effective and easy models for donor-acceptor dyes accounting for a single coupled vibration.

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