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Computational Investigation of the Spin-Density Asymmetry in Photosynthetic Reaction Center Models from First Principles

revised on 29.03.2020, 13:25 and posted on 31.03.2020, 06:21 by Denis Artiukhin, Patrick Eschenbach, Johannes Neugebauer
We present a computational analysis of the spin-density asymmetry in cation radical states of reaction center models from photosystem I, photosystem II, and bacteria from Synechococcus elongatus, Thermococcus vulcanus, and Rhodobacter sphaeroides, respectively. The recently developed FDE-diab methodology [J. Chem. Phys., 148 (2018), 214104] allowed us to effectively avoid the spin-density overdelocalization error characteristic for standard Kohn–Sham Density Functional Theory and to reliably calculate spin-density distributions and electronic couplings for a number of molecular systems ranging from inner pairs of (bacterio)chlorophyll a molecules in vacuum to large protein including up to about 2000 atoms. The calculated spin densities show a good agreement with available experimental results and were used to validate reaction center models reported in the literature. Here we demonstrate that the applied theoretical approach is very sensitive to changes in molecular structures and relative orientation of molecules. This makes FDE-diab a valuable tool for electronic structure calculations of large photosynthetic models effectively complementing the existing experimental techniques.


EU Horizon 2020 research and innovation programme


Email Address of Submitting Author


Department of Chemistry, Aarhus Universitet



ORCID For Submitting Author


Declaration of Conflict of Interest

The Authors declare that there is no conflict of interest.

Version Notes

version 29.03.20