Energy transfer pathways in light-harvesting complexes of purple bacteria as revealed by global kinetic analysis of two-dimensional transient spectra

J Phys Chem B. 2013 Sep 26;117(38):11349-62. doi: 10.1021/jp403028x. Epub 2013 Jul 18.

Abstract

Excited state dynamics in LH2 complexes of two purple bacterial species were studied by broad-band two-dimensional electronic spectroscopy. The optical response was measured in the 500-600 nm spectral region on the 0-400 fs time scale. Global target analysis of two-dimensional (2D) transient spectra revealed the main energy transfer pathways between carotenoid S2, 1Bu(-) and S1 states and bacteriochlorophyll Qx state. Global analysis ascertained the evolutionary and vibration-associated spectra, which also indicated the presence of a higher-lying vibrational level in the carotenoid S1 state. The estimation of the spectral overlap between the 1Bu(-) state and the Qx state indicated a significant contribution of the 1Bu(-) state to the overall S2-to-Qx excitation energy transfer.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Bacterial Proteins / chemistry*
  • Bacterial Proteins / metabolism
  • Bacteriochlorophylls / chemistry
  • Carotenoids / chemistry
  • Energy Transfer
  • Kinetics
  • Light-Harvesting Protein Complexes / chemistry*
  • Light-Harvesting Protein Complexes / metabolism
  • Photoelectron Spectroscopy
  • Proteobacteria / metabolism*
  • Rhodobacter / metabolism
  • Rhodopseudomonas / metabolism
  • Time Factors

Substances

  • Bacterial Proteins
  • Bacteriochlorophylls
  • Light-Harvesting Protein Complexes
  • Carotenoids