Directed ultrafast conformational changes accompany electron transfer in a photolyase as resolved by serial crystallography-Reference-Cited by-同舟云学术

Directed ultrafast conformational changes accompany electron transfer in a photolyase as resolved by serial crystallography

Published:2024-01-15 Issue: Volume: Page:
ISSN:1755-4330
Container-title:Nature Chemistry
language:en
Short-container-title:Nat. Chem.

Author:

Cellini Andrea^ORCID,Shankar Madan Kumar^ORCID,Nimmrich Amke^ORCID,Hunt Leigh Anna^ORCID,Monrroy Leonardo^ORCID,Mutisya Jennifer,Furrer Antonia,Beale Emma V.^ORCID,Carrillo Melissa^ORCID,Malla Tek Narsingh^ORCID,Maj Piotr^ORCID,Vrhovac Lidija^ORCID,Dworkowski Florian^ORCID,Cirelli Claudio^ORCID,Johnson Philip J. M.^ORCID,Ozerov Dmitry^ORCID,Stojković Emina A.^ORCID,Hammarström Leif^ORCID,Bacellar Camila^ORCID,Standfuss Jörg^ORCID,Maj Michał^ORCID,Schmidt Marius^ORCID,Weinert Tobias^ORCID,Ihalainen Janne A.^ORCID,Wahlgren Weixiao Yuan,Westenhoff Sebastian^ORCID

Abstract

AbstractCharge-transfer reactions in proteins are important for life, such as in photolyases which repair DNA, but the role of structural dynamics remains unclear. Here, using femtosecond X-ray crystallography, we report the structural changes that take place while electrons transfer along a chain of four conserved tryptophans in the Drosophila melanogaster (6-4) photolyase. At femto- and picosecond delays, photoreduction of the flavin by the first tryptophan causes directed structural responses at a key asparagine, at a conserved salt bridge, and by rearrangements of nearby water molecules. We detect charge-induced structural changes close to the second tryptophan from 1 ps to 20 ps, identifying a nearby methionine as an active participant in the redox chain, and from 20 ps around the fourth tryptophan. The photolyase undergoes highly directed and carefully timed adaptations of its structure. This questions the validity of the linear solvent response approximation in Marcus theory and indicates that evolution has optimized fast protein fluctuations for optimal charge transfer.

Publisher

Springer Science and Business Media LLC

Subject

General Chemical Engineering,General Chemistry

Link

https://www.nature.com/articles/s41557-023-01413-9.pdf

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