Energy transfer under natural incoherent light: Effects of asymmetry on efficiency

Abstract

The non-equilibrium stationary coherences that form in donor–acceptor systems are investigated to determine their relationship to the efficiency of energy transfer to a neighboring reaction center. It is found that the effects of asymmetry in the dimer are generally detrimental to the transfer of energy. Four types of systems are examined, arising from combinations of localized trapping, delocalized (Forster) trapping, eigenstate dephasing, and site basis dephasing. In the cases of site basis dephasing, the interplay between the energy gap of the excited dimer states and the environment is shown to give rise to a turnover effect in the efficiency under weak dimer coupling conditions. Furthermore, the nature of the coherences and associated flux is interpreted in terms of pathway interference effects. In addition, regardless of the cases considered, the ratio of the real part and the imaginary part of the coherences in the energy-eigenbasis tends to a constant value in the steady state limit.

Document Details

Document Type
Pub Defense Publication
Publication Date
Sep 15, 2020
Source ID
10.1063/5.0020576

Entities

People

  • Kenneth A Jung
  • Paul Brumer

Organizations

  • Air Force Office of Scientific Research
  • University of Toronto

Tags

Fields of Study

  • Physics

Readers

  • Molecular Photonics/Laser Physics
  • Quantum spin resonance or Electron Paramagnetic Resonance spectroscopy.
  • Systems Analysis and Design