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In this paper we work out a parameterization of the environment noise withinthe Haken-Strobl-Reinenker (HSR) model for the PE545 light-harvesting complexbased on atomic-level quantum mechanics/molecular mechanics (QM/MM)simulations. We use this approach to investigate the role of different auto-and cross-correlations in the HSR noise tensor, confirming that site-energyautocorrelations (pure dephasing) terms dominate the noise-induced excitonmobility enhancement, followed by site energy-coupling cross-correlations forspecific triplets of pigments. Interestingly, several cross-correlations of thelatter kind, together with coupling-coupling cross-correlations, display clearlow-frequency signatures in their spectral densities in the region 30-70inverse centimeters. These slow components lie at the limits of validity of theHSR approach, requiring that environmental fluctuations be faster than typicalexciton transfer time scales. We show that a simple coarse-grainedelastic-network-model (ENM) analysis of the PE545 protein naturally spotlightscollective normal modes in this frequency range, that represent specificconcerted motions of the subnetwork of cysteines that are covalenty linked tothe pigments. This analysis strongly suggests that protein scaffolds inlight-harvesting complexes are able to express specific collective,low-frequency normal modes providing a fold-rooted blueprint of excitontransport pathways. We speculate that ENM-based mixed quantum classicalmethods, such as Ehrenfest dynamics, might be promising tools to disentanglethe fundamental designing principles of these dynamical processes in naturaland artificial light-harvesting structures.

Exciton transport in the PE545 complex: insight from atomistic QM/MM-based quantum master equations and elastic network models