Time-Domain Line-Shape Analysis from 2D Spectroscopy to Precisely Determine Hamiltonian Parameters for a Photosynthetic Complex

J Phys Chem B. 2021 Mar 25;125(11):2812-2820. doi: 10.1021/acs.jpcb.0c08012. Epub 2021 Mar 17.

Abstract

Optical signals come from coherences between quantum states, with spectral line widths determined by the coherences' dephasing dynamics. Using a 2D electronic spectrometer, we observe weak coherence- and rephasing-time-domain signals persisting to 1 ps in the Fenna-Matthews-Olson complex at 77 K. These are coherences between the ground and excited states prepared after the complex interacts once or three times with light, rather than zero-quantum coherences that are more frequently investigated following two interactions. Here, we use these small but persistent signal components to isolate spectral contributions with narrowed peaks and reveal the system's eigenenergies.

Publication types

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

MeSH terms

  • Light-Harvesting Protein Complexes*
  • Photosynthetic Reaction Center Complex Proteins*
  • Quantum Theory
  • Spectrum Analysis

Substances

  • Light-Harvesting Protein Complexes
  • Photosynthetic Reaction Center Complex Proteins