Structural basis of the radical pair state in photolyases and cryptochromes

Andrea Cellini; Madan Kumar Shankar; Weixiao Yuan Wahlgren; Amke Nimmrich; Antonia Furrer; Daniel James; Maximilian Wranik; Sylvain Aumonier; Emma V. Beale; Florian Dworkowski; Jörg Standfuss; Tobias Weinert; Sebastian Westenhoff

doi:10.1039/D2CC00376G

Structural basis of the radical pair state in photolyases and cryptochromes†

Andrea Cellini,

^a Madan Kumar Shankar,

^a Weixiao Yuan Wahlgren,^a Amke Nimmrich,^a Antonia Furrer,

^b Daniel James,^b Maximilian Wranik,^b Sylvain Aumonier,^c Emma V. Beale,

^d Florian Dworkowski,

^c Jörg Standfuss,^b Tobias Weinert^b and Sebastian Westenhoff

*^ae

Author affiliations

* Corresponding authors

^a Department of Chemistry and Molecular Biology, University of Gothenburg, Box 462, 40530 Gothenburg, Sweden
E-mail: westenho@chem.gu.se

^b Division of Biology and Chemistry-Laboratory for Biomolecular Research, Paul Scherrer Institut, 5232 Villigen, Switzerland

^c Photon Science Division – Laboratory for Macromolecules and Bioimaging (LSB), Paul Scherrer Institut, 5232 Villigen, Switzerland

^d Photon Science Division – Laboratory for Synchrotron Radiation and Femtochemistry (LSF), Paul Scherrer Institut, 5232 Villigen, Switzerland

^e Department of Chemistry-BMC, University of Uppsala, Husargatan 3, 75237 Uppsala, Sweden

Abstract

We present the structure of a photoactivated animal (6-4) photolyase in its radical pair state, captured by serial crystallography. We observe how a conserved asparigine moves towards the semiquinone FAD chromophore and stabilizes it by hydrogen bonding. Several amino acids around the final tryptophan radical rearrange, opening it up to the solvent. The structure explains how the protein environment stabilizes the radical pair state, which is crucial for function of (6-4) photolyases and cryptochromes.

Chemical Communications

Structural basis of the radical pair state in photolyases and cryptochromes†

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Structural basis of the radical pair state in photolyases and cryptochromes

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