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Area of Science:

  • Physical Chemistry
  • Spectroscopy
  • Biophysics

Background:

  • Two-dimensional coherent electronic spectroscopy (2DES) is crucial for dissecting spectral line shape contributions from homogeneous and inhomogeneous broadening.
  • Environmental fluctuations significantly impact molecular transition spectra, influencing spectral line shapes.

Purpose of the Study:

  • To investigate the nature of protein environment fluctuations affecting molecular transitions using 2DES.
  • To determine if a harmonic environmental model is suitable for describing pigment dynamics in LH2 aggregates at different temperatures.

Main Methods:

  • Utilized an excitonic model of a double-ring LH2 aggregate.
  • Performed simulations of 2DES spectra for the LH2 aggregate.
  • Analyzed spectral line shapes to distinguish between homogeneous and inhomogeneous broadening.

Main Results:

  • A harmonic environmental model failed to yield consistent parameters for the B850 ring pigments at 77 K and room temperature.
  • Simulations indicated that protein fluctuations for the B850 ring pigments are highly anharmonic.
  • Fluctuations for the B800 ring pigments could be adequately described by a harmonic model within the studied temperature range.

Conclusions:

  • The study highlights the anharmonic nature of protein environment fluctuations impacting B850 ring pigments in LH2 aggregates.
  • Findings suggest that different pigment sites within an aggregate can exhibit distinct environmental dynamics.
  • The results underscore the importance of considering anharmonicity in environmental models for accurate spectral interpretation.