On the Exciton Coupling between Two Chlorophyll Pigments in the Absence of a Protein Environment: Intrinsic Effects Revealed by Theory and Experiment (German ed)

Abstract

Exciton coupling between two or more chlorophyll (Chl) pigments is a key mechanism associated with the color tuning of photosynthetic proteins but it is difficult to disentangle this effect from shifts that are due to the protein microenvironment. Herein, we report the formation of the simplest coupled system, the Chl a dimer, tagged with a quaternary ammonium ion by electrospray ionization. Based on action spectroscopic studies in vacuo, the dimer complexes were found to absorb 5070 meV to the red of the monomers under the same conditions. First-principles calculations predict shifts that somewhat depend on the relative orientation of the two Chl units, namely 50 and 30 meV for structures where the Chl rings are stacked and unstacked, respectively. Our work demonstrates that Chl association alone can produce a large portion of the color shift observed in photosynthetic macromolecular assemblies.

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Document Details

Document Type
Technical Report
Publication Date
Jul 29, 2016
Accession Number
AD1010032

Entities

People

  • Bruce F Milne
  • Christina Kjr
  • Jrgen Houmller
  • Mark H. Stockett
  • Steen B. Nielsen
  • Yoni Toker
  • Ángel Rubio Secades

Organizations

  • University of Coimbra

Tags

Communities of Interest

  • Energy and Power Technologies

DTIC Thesaurus Topics

  • Absorption
  • Absorption Spectra
  • Advanced Materials
  • Chromophores
  • Computational Science
  • Density Functional Theory
  • Dissociation
  • Electrospray Ionization
  • Energy
  • Energy Transfer
  • Lasers
  • Light Sources
  • Mass Spectra
  • Mass Spectrometry
  • Pigments
  • Spectra
  • Spectroscopy

Readers

  • Chemistry (specifically Chemical Fluorescence)
  • Molecular and Cellular Biochemistry
  • Structural Dynamics.

Technology Areas

  • Microelectronics