ArticleJournal of the American Chemical Society2012
Electron tunneling pathways and role of adenine in repair of cyclobutane pyrimidine dimer by DNA photolyase.
Article in Journal of the American Chemical Society, 2012. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 27 papers.
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Who cites it
27 citing papers in PubMed, 64 citations in OpenAlex.
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- Elucidation of a distinct photoreduction pathway in class IIProceedings of the National Academy of Sciences of the United States of America · 2025Article
- Tunneling Times in an Asymmetric Harmonic Double-Well with Application to Electron Transfers in Biological Macromolecules.ACS omega · 2024Article
- Dynamics and mechanism of DNA repair by a bifunctional cryptochrome.Proceedings of the National Academy of Sciences of the United States of America · 2024Article
- DNA damage repair: historical perspectives, mechanistic pathways and clinical translation for targeted cancer therapy.Signal transduction and targeted therapy · 2021Review
- Active-Site Environmental Factors Customize the Photophysics of Photoenzymatic Old Yellow Enzymes.The journal of physical chemistry. B · 2020Article
- Nonequilibrium dynamics of photoinduced forward and backward electron transfer reactions.The Journal of chemical physics · 2020Article
- Theoretical insights into the DNA repair function ofBiophysics and physicobiology · 2020Article
- Understanding Short-Range Electron-Transfer Dynamics in Proteins.The journal of physical chemistry letters · 2019Article
- Distinct properties underlie flavin-based electron bifurcation in a novel electron transfer flavoprotein FixAB fromThe Journal of biological chemistry · 2018Article
- Determinants of Photolyase's DNA Repair Mechanism in Mesophiles and Extremophiles.Journal of the American Chemical Society · 2018Article
- The binding structure and affinity of photodamaged duplex DNA with members of the photolyase/cryptochrome family: A computational study.Biophysics and physicobiology · 2018Article
- 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
- An Ethenoadenine FAD Analog Accelerates UV Dimer Repair by DNA Photolyase.Photochemistry and photobiology · 2017Article
- 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
- Synthesis and application of isotopically labeled flavin nucleotides.Journal of labelled compounds & radiopharmaceuticals · 2015Article
- The molecular origin of high DNA-repair efficiency by photolyase.Nature communications · 2015Article
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Authors and funding
8 authors at 2 institutions in 1 country.
Funding
Abstract
Electron tunneling pathways in enzymes are critical to their catalytic efficiency. Through electron tunneling, photolyase, a photoenzyme, splits UV-induced cyclobutane pyrimidine dimer into two normal bases. Here, we report our systematic characterization and analyses of photoinitiated three electron transfer processes and cyclobutane ring splitting by following the entire dynamical evolution during enzymatic repair with femtosecond resolution. We observed the complete dynamics of the reactants, all intermediates and final products, and determined their reaction time scales. Using (deoxy)uracil and thymine as dimer substrates, we unambiguously determined the electron tunneling pathways for the forward electron transfer to initiate repair and for the final electron return to restore the active cofactor and complete the catalytic photocycle. Significantly, we found that the adenine moiety of the unusual bent flavin cofactor is essential to mediating all electron-transfer dynamics through a superexchange mechanism, leading to a delicate balance of time scales. The cyclobutane ring splitting takes tens of picoseconds, while electron-transfer dynamics all occur on a longer time scale. The active-site structural integrity, unique electron tunneling pathways, and the critical role of adenine ensure the synergy of these elementary steps in this complex photorepair machinery to achieve maximum repair efficiency which is close to unity. Finally, we used the Marcus electron-transfer theory to evaluate all three electron-transfer processes and thus obtained their reaction driving forces (free energies), reorganization energies, and electronic coupling constants, concluding that the forward and futile back-electron transfer is in the normal region and that the final electron return of the catalytic cycle is in the inverted region.
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Registered trials
Read under generation 80e0d062 · epoch 390. Bibliography from PubMed, PubMed Central and OpenAlex; grants from NIH RePORTER; trial links from ClinicalTrials.gov; estimates, votes and beliefs from the OpenQuestion graph.