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Spatial and Electronic Correlations in the PE545 Light-Harvesting Complex.
Lucas Viani1, Carles Curutchet2, Benedetta Mennucci1
1†Dipartimento di Chimica e Chimica Industriale, Università di Pisa, via Risorgimento 35, 56126 Pisa, Italy.
The Journal of Physical Chemistry Letters
|August 19, 2015
Summary
Quantum coherence in photosynthesis is influenced by protein and water dynamics. Phycobiliproteins exhibit unique energy correlations, enhancing light-harvesting efficiency compared to chlorophyll complexes.
Area of Science:
- Photosynthetic light-harvesting
- Quantum biology
- Biophysics
Background:
- Long-lasting quantum coherence effects observed in photosynthetic pigment-protein complexes challenge existing models.
- Protein motions are increasingly recognized for their role in light-harvesting processes.
- Correlated fluctuations in pigment site energies and couplings are hypothesized to explain these quantum effects.
Purpose of the Study:
- To investigate the degree of correlated fluctuations in the PE545 complex of Rhodomonas sp.
- To analyze the interplay between chromophore motions, water solvent, and energy correlations.
- To compare the observed correlations with those in other light-harvesting complexes like the Fenna-Matthews-Olson complex.
Main Methods:
- Combined molecular dynamics (MD) simulations and quantum mechanics/molecular mechanics (QM/MM) calculations.
- Analysis of correlated fluctuations in chromophore motions and their impact on site energies and couplings.
- Comparative analysis with existing data from other pigment-protein complexes.
Main Results:
- Correlations between chromophore motions, significantly influenced by the water solvent, were identified.
- These motions did not result in substantial site energy correlations.
- Significant cross-correlations between energies and couplings were observed in the PE545 complex.
Conclusions:
- The PE545 complex exhibits distinct energy and coupling correlations compared to chlorophyll-based complexes.
- Water solvent plays a crucial role in mediating chromophore motion correlations.
- Phycobiliproteins may possess a unique mechanism for controlling quantum coherence and light-harvesting efficiency.
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