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Issue 31, 2019
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Biological relevance of charge transfer branching pathways in photolyases

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Abstract

The repair of sun-induced DNA lesions by photolyases is driven by a photoinduced electron transfer from a fully reduced FAD to the damaged DNA. A chain of several aromatic residues connecting FAD to solvent ensures the prior photoreduction of the FAD cofactor. In PhrA, a class III CPD photolyase, two branching tryptophan charge transfer pathways have been characterized. According to previous experiments, both pathways play a role in the FAD photoreduction. To provide a molecular insight to the charge transfer abilities of both pathways, we perform multiscales simulations where the protein motion and the positive charge are simultaneously propagated. Our computational approach reveals that one pathway drives a very fast charge transfer whereas the other pathway provides a very good thermodynamic stabilization of the positive charge. During the simulations, the positive charge firstly moves on the fast triad, while a reorganization of the close FAD˙ environment occurs. Then, backward transfers can lead to the propagation of the positive charge on the second pathway. After one nanosecond, we observe a nearly equal probability to find the charge at ending tryptophan of either pathway; eventually the charge distribution will likely evolve towards a charge stabilization on the last tryptophan of the slowest pathway. Our results highlight the role the protein environment, which manages the association of a kinetic and a thermodynamic pathways to trigger a fast and efficient FAD photoreduction.

Graphical abstract: Biological relevance of charge transfer branching pathways in photolyases

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Publication details

The article was received on 21 Mar 2019, accepted on 09 Jul 2019 and first published on 10 Jul 2019


Article type: Paper
DOI: 10.1039/C9CP01609K
Phys. Chem. Chem. Phys., 2019,21, 17072-17081
  • Open access: Creative Commons BY-NC license
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    Biological relevance of charge transfer branching pathways in photolyases

    D. Holub, T. Lamparter, M. Elstner and N. Gillet, Phys. Chem. Chem. Phys., 2019, 21, 17072
    DOI: 10.1039/C9CP01609K

    This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Material from this article can be used in other publications provided that the correct acknowledgement is given with the reproduced material and it is not used for commercial purposes.

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      [Original citation] - Published by The Royal Society of Chemistry (RSC) on behalf of the European Society for Photobiology, the European Photochemistry Association, and RSC.
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      [Original citation] - Published by The Royal Society of Chemistry.

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