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- W4232924871 abstract "One of the detrimental effects of ultraviolet radiation on DNA is the formation of the (6-4) photoproduct, 6-4PP, between two adjacent pyrimidine rings. This lesion interferes with replication and transcription, and may result in mutation and cell death. In many organisms, a flavoenzyme called photolyase uses blue light energy to repair the 6-4PP (ref. 3). The molecular mechanism of the repair reaction is poorly understood. Here, we use ultrafast spectroscopy to show that the key step in the repair photocycle is acyclic proton transfer between the enzyme and the substrate. By femtosecond synchronization of the enzymatic dynamics with the repair function, we followed the function evolution and observed direct electron transfer from the excited flavin cofactor to the 6-4PP in 225 picoseconds, but surprisingly fast back electron transfer in 50 picoseconds without repair. We found that the catalytic proton transfer between a histidine residue in the active site and the 6-4PP, induced by the initial photoinduced electron transfer from the excited flavin cofactor to 6-4PP, occurs in 425 picoseconds and leads to 6-4PP repair in tens of nanoseconds. These key dynamics define the repair photocycle and explain the underlying molecular mechanism of the enzyme's modest efficiency. PMID: 20657578 Funding information This work was supported by: NLM NIH HHS, United States Grant ID: R01 LM006845 NHGRI NIH HHS, United States Grant ID: R01 HG002779-06 NHGRI NIH HHS, United States Grant ID: R01 HG002779-05 NIGMS NIH HHS, United States Grant ID: R01 GM074813-04 NIGMS NIH HHS, United States Grant ID: R01 GM074813 NIGMS NIH HHS, United States Grant ID: R01 GM031082 NIEHS NIH HHS, United States Grant ID: P30 ES010126 NIGMS NIH HHS, United States Grant ID: GM074813 More Less keyboard_arrow_down" @default.
- W4232924871 created "2022-05-12" @default.
- W4232924871 creator A5062585452 @default.
- W4232924871 date "2010-07-27" @default.
- W4232924871 modified "2023-09-27" @default.
- W4232924871 title "Faculty Opinions recommendation of Dynamics and mechanism of repair of ultraviolet-induced (6-4) photoproduct by photolyase." @default.
- W4232924871 doi "https://doi.org/10.3410/f.4390972.4221072" @default.
- W4232924871 hasPublicationYear "2010" @default.
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