2020, Chaillet, Martin L., Lengauer, Florian, Adolphs, Julian, Müh, Frank, Fokas, Alexander S., Cole, Daniel J., Chin, Alex W., Renger, Thomas

Inhomogeneous broadening of optical lines of the Fenna-Matthews-Olson (FMO) light-harvesting protein is investigated by combining a Monte Carlo sampling of low-energy conformational substates of the protein with a quantum chemical/electrostatic calculation of local transition energies (site energies) of the pigments. The good agreement between the optical spectra calculated for the inhomogeneous ensemble and the experimental data demonstrates that electrostatics is the dominant contributor to static disorder in site energies. Rotamers of polar amino acid side chains are found to cause bimodal distribution functions of site energy shifts, which can be probed by hole burning and single-molecule spectroscopy. When summing over the large number of contributions, the resulting distribution functions of the site energies become Gaussians, and the correlations in site energy fluctuations at different sites practically average to zero. These results demonstrate that static disorder in the FMO protein is in the realm of the central limit theorem of statistics. © 2020 American Chemical Society.

2017, Schultz, P., Menck, P.J., Heitzig, J., Kurths, J.

Stability assessment methods for dynamical systems have recently been complemented by basin stability and derived measures, i.e. probabilistic statements whether systems remain in a basin of attraction given a distribution of perturbations. Their application requires numerical estimation via Monte Carlo sampling and integration of differential equations. Here, we analyse the applicability of basin stability to systems with basin geometries that are challenging for this numerical method, having fractal basin boundaries and riddled or intermingled basins of attraction. We find that numerical basin stability estimation is still meaningful for fractal boundaries but reaches its limits for riddled basins with holes.