Multi-layer multi-configuration time-dependent Hartree (ML-MCTDH) approach to the correlated exciton-vibrational dynamics in the FMO complex

Jan Schulze, Mohamed F. Shibl, Jaber Al Marri, Oliver K�hn

Research output: Contribution to journalArticle

31 Citations (Scopus)

Abstract

The coupled quantum dynamics of excitonic and vibrational degrees of freedom is investigated for high-dimensional models of the Fenna-Matthews-Olson complex. This includes a seven- and an eight-site model with 518 and 592 harmonic vibrational modes, respectively. The coupling between local electronic transitions and vibrations is described within the Huang-Rhys model using parameters that are obtained by discretization of an experimental spectral density. Different pathways of excitation energy flow are analyzed in terms of the reduced one-exciton density matrix, focussing on the role of vibrational and vibronic excitations. Distinct features due to both competing time scales of vibrational and exciton motion and vibronically assisted transfer are observed. The question of the effect of initial state preparation is addressed by comparing the case of an instantaneous Franck-Condon excitation at a single site with that of a laser field excitation.

Original languageEnglish
Article number185101
JournalJournal of Chemical Physics
Volume144
Issue number18
DOIs
Publication statusPublished - 14 May 2016
Externally publishedYes

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excitons
configurations
excitation
Excitation energy
Spectral density
Degrees of freedom (mechanics)
vibration mode
Lasers
degrees of freedom
harmonics
vibration
preparation
LDS 751
electronics
lasers
energy

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Multi-layer multi-configuration time-dependent Hartree (ML-MCTDH) approach to the correlated exciton-vibrational dynamics in the FMO complex. / Schulze, Jan; Shibl, Mohamed F.; Al Marri, Jaber; K�hn, Oliver.

In: Journal of Chemical Physics, Vol. 144, No. 18, 185101, 14.05.2016.

Research output: Contribution to journalArticle

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