Multiphonon transitions in the biomolecular energy transfer dynamics

Link:
Autor/in:
Erscheinungsjahr:
2010
Medientyp:
Text
Schlagworte:
  • Excitons
  • Energy transfer
  • FMO complex
  • Photosystem II Protein Complex
  • Photosynthesis
  • Chlorophyll
  • Excitons
  • Energy transfer
  • FMO complex
  • Photosystem II Protein Complex
  • Photosynthesis
  • Chlorophyll
Beschreibung:
  • We show that the biomolecular exciton dynamics under the influence of slow polarization fluctuations in the solvent cannot be described by lowest order, one-phonon approaches which are perturbative in the system-bath coupling. Instead, nonperturbative multiphonon transitions induced by the slow bath yield significant contributions. This is shown by comparing results for the decoherence rate of the exciton dynamics of a resumed perturbation theory with numerically exact real-time path-integral data. The exact decoherence rate for realistically slow solvent environments is significantly modified by multiphonon processes even in the weak coupling regime, while a one-phonon description is satisfactory only for fast environmental noise. Slow environments inhibit bath modes that are resonant with the exciton dynamics, thereby suppressing one-phonon transitions and enhancing multiphonon processes, which are typically not captured by lowest order perturbative treatments, such as Redfield or Lindblad approaches, even in more refined variants.
Lizenz:
  • info:eu-repo/semantics/restrictedAccess
Quellsystem:
Forschungsinformationssystem der UHH

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oai:www.edit.fis.uni-hamburg.de:publications/951c4ec3-ba1a-4c43-8d88-8959f0843981