Hydrogen Bonding Environments in the Photocycle Process around the Flavin Chromophore of the AppA-BLUF domain

Journal of the American Chemical Society
Tatsuya IwataHideki Kandori

Abstract

Three kinds of photochemical reactions are known in flavins as chromophores of photosensor proteins, reflecting the various catalytic reactions of the flavin in flavoenzymes. Sensor of blue light using the flavin FAD (BLUF) domains exhibit a unique photoreaction compared with other flavin-binding photoreceptors in that the chromophore does not change its chemical structure between unphotolyzed and intermediate states. Rather, the hydrogen bonding environment is altered, whereby the conserved Gln and Tyr residues near FAD play a crucial role. One proposal for this behavior is that the conserved Gln changes its chemical structure from a keto to an enol. We applied light-induced difference Fourier transform infrared (FTIR) spectroscopy to AppA-BLUF. The spectra of AppA-BLUF exhibited a different feature upon 15N-Gln labeling compared with the previously reported spectra from BlrB, a different BLUF domain. The FTIR signals were interpreted from quantum mechanics/molecular mechanics (QM/MM) calculation as the keto-enol tautomerization and rotation of the Gln63 side chain in the AppA-BLUF domain. The former was consistent with the result from BlrB, but the latter was not uniquely determined by the previous study. QM/MM calculation al...Continue Reading

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Citations

Jun 25, 2020·Nature Communications·Andreas GramlBurkhard König
Mar 24, 2020·Chemical Reviews·Victor A Lorenz-Fonfria
Mar 7, 2021·Journal of Computational Chemistry·Elena O LevinaVladimir G Tsirelson
Jun 19, 2021·Physical Chemistry Chemical Physics : PCCP·Prokopis C AndrikopoulosGustavo Fuertes
Jul 6, 2021·Spectrochimica Acta. Part A, Molecular and Biomolecular Spectroscopy·Mohammad Pabel KabirSamer Gozem
Jun 29, 2021·Biophysics and Physicobiology·Masashi UnnoJun Tamogami
Dec 26, 2018·Journal of the American Chemical Society·Alireza GhanbarpourJames H Geiger
Oct 10, 2019·The Journal of Physical Chemistry. B·Christopher R HallStephen R Meech
Jan 13, 2022·Accounts of Chemical Research·Andras LukacsStephen R Meech
Dec 21, 2021·Angewandte Chemie·Xiu-Wen KangDongping Zhong

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