Two-dimensional electronic spectroscopy of the B800-B820 light-harvesting complex

Research output: Contribution to journalArticle

Abstract

Emerging nonlinear optical spectroscopies enable deeper insight into the intricate world of interactions and dynamics of complex molecular systems. 2D electronic spectroscopy appears to be especially well suited for studying multichromophoric complexes such as light-harvesting complexes of photosynthetic organisms as it allows direct observation of couplings between the pigments and charts dynamics of energy flow on a 2D frequency map. Here, we demonstrate that a single 2D experiment combined with self-consistent theoretical modeling can determine spectroscopic parameters dictating excitation energy dynamics in the bacterial B800-B820 light-harvesting complex, which contains 27 bacteriochlorophyll molecules. Ultrafast sub-50-fs dynamics dominated by coherent intraband processes and population transfer dynamics on a picosecond time scale were measured and modeled with one consistent set of parameters. Theoretical 2D spectra were calculated by using a Frenkel exciton model and modified Forster/Redfield theory for the calculation of dynamics. They match the main features of experimental spectra at all population times well, implying that the energy level structure and transition dipole strengths are modeled correctly in addition to the energy transfer dynamics of the system.

Details

Authors
  • Donatas Zigmantas
  • E. L. Read
  • T. Mancal
  • T. Brixner
  • A. T. Gardiner
  • R. J. Cogdell
  • G. R. Fleming
External organisations
  • External Organization - Unknown
Research areas and keywords

Subject classification (UKÄ) – MANDATORY

  • Atom and Molecular Physics and Optics

Keywords

  • photosynthetic complexes, multichromophoric systems, ultrafast spectroscopy, photosynthetic purple bacteria, excitation-energy transfer, echo peak shift, femtosecond spectroscopy, room-temperature, transfer dynamics, lh2, antenna system, couplings, acidophila, excitons
Original languageEnglish
Pages (from-to)12672-12677
JournalProceedings of the National Academy of Sciences
Volume103
Issue number34
Publication statusPublished - 2006
Publication categoryResearch
Peer-reviewedYes
Externally publishedYes

Bibliographic note

The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)