ArticleProceedings of the National Academy of Sciences of the United States of America2013
Dynamic determination of the functional state in photolyase and the implication for cryptochrome.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 23 papers.
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Who cites it
23 citing papers in PubMed, 53 citations in OpenAlex.
- On the Origin of the Red-Shifted Flavin Absorption Spectra in Fatty Acid Photodecarboxylase.The journal of physical chemistry. B · 2026Article
- The ionic and protonation states of flavin control the activation and recovery of Drosophila cryptochrome.Communications chemistry · 2025Article
- Dynamics and mechanism of DNA repair by a bifunctional cryptochrome.Proceedings of the National Academy of Sciences of the United States of America · 2024Article
- Ultrafast Dynamics and Catalytic Mechanism of Fatty Acid Photodecarboxylase.Angewandte Chemie (International ed. in English) · 2022Article
- Ultrafast Dynamics of Fatty Acid Photodecarboxylase in Anionic Semiquinone State.The journal of physical chemistry letters · 2022Article
- Activation mechanism ofScience advances · 2021Article
- Identification of the vibrational marker of tyrosine cation radical using ultrafast transient infrared spectroscopy of flavoprotein systems.Photochemical & photobiological sciences : Official journal of the European Photochemistry Association and the European Society for Photobiology · 2021Article
- A topologically distinct class of photolyases specific for UV lesions within single-stranded DNA.Nucleic acids research · 2020Article
- Light-induced chromophore and protein responses and mechanical signal transduction of BLUF proteins.Biophysical reviews · 2018Review
- Photolyase: Dynamics and electron-transfer mechanisms of DNA repair.Archives of biochemistry and biophysics · 2017Review
- Photolyase: Dynamics and Mechanisms of Repair of Sun-Induced DNA Damage.Photochemistry and photobiology · 2017Review
- Overlapping Electronic States with Nearly Parallel Transition Dipole Moments in Reduced Anionic Flavin Can Distort Photobiological Dynamics.Journal of the American Chemical Society · 2016Article
- Bifurcating electron-transfer pathways in DNA photolyases determine the repair quantum yield.Science (New York, N.Y.) · 2016Article
- Characterization of the Intermediate in and Identification of the Repair Mechanism of (6-4) Photolesions by Photolyases.Angewandte Chemie (International ed. in English) · 2016Article
- The molecular origin of high DNA-repair efficiency by photolyase.Nature communications · 2015Article
- Dynamics and mechanisms of DNA repair by photolyase.Physical chemistry chemical physics : PCCP · 2015Review
- Direct determination of resonance energy transfer in photolyase: structural alignment for the functional state.The journal of physical chemistry. A · 2014Article
- Photochemistry of flavoprotein light sensors.Nature chemical biology · 2014Review
- ATP binding turns plant cryptochrome into an efficient natural photoswitch.Scientific reports · 2014Article
- Dynamic Determination of Active-Site Reactivity in Semiquinone Photolyase by the Cofactor Photoreduction.The journal of physical chemistry letters · 2014Article
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Authors and funding
8 authors at 2 institutions in 1 country.
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Abstract
The flavin adenine dinucleotide cofactor has an unusual bent configuration in photolyase and cryptochrome, and such a folded structure may have a functional role in initial photochemistry. Using femtosecond spectroscopy, we report here our systematic characterization of cyclic intramolecular electron transfer (ET) dynamics between the flavin and adenine moieties of flavin adenine dinucleotide in four redox forms of the oxidized, neutral, and anionic semiquinone, and anionic hydroquinone states. By comparing wild-type and mutant enzymes, we have determined that the excited neutral oxidized and semiquinone states absorb an electron from the adenine moiety in 19 and 135 ps, whereas the excited anionic semiquinone and hydroquinone states donate an electron to the adenine moiety in 12 ps and 2 ns, respectively. All back ET dynamics occur ultrafast within 100 ps. These four ET dynamics dictate that only the anionic hydroquinone flavin can be the functional state in photolyase due to the slower ET dynamics (2 ns) with the adenine moiety and a faster ET dynamics (250 ps) with the substrate, whereas the intervening adenine moiety mediates electron tunneling for repair of damaged DNA. Assuming ET as the universal mechanism for photolyase and cryptochrome, these results imply anionic flavin as the more attractive form of the cofactor in the active state in cryptochrome to induce charge relocation to cause an electrostatic variation in the active site and then lead to a local conformation change to initiate signaling.
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