ArticleProceedings of the National Academy of Sciences of the United States of America2010
Ultrafast solvation dynamics at binding and active sites of photolyases.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2010. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 30 papers.
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Who cites it
30 citing papers in PubMed.
- Ultrafast Dynamics and Catalytic Mechanism of Fatty Acid Photodecarboxylase.Angewandte Chemie (International ed. in English) · 2022Article
- What Does Time-Dependent Fluorescence Shift (TDFS) in Biomembranes (and Proteins) Report on?Frontiers in chemistry · 2021Review
- Revealing the origin of multiphasic dynamic behaviors in cyanobacteriochrome.Proceedings of the National Academy of Sciences of the United States of America · 2020Article
- The Origin of Ultrafast Multiphasic Dynamics in Photoisomerization of Bacteriophytochrome.The journal of physical chemistry letters · 2020Article
- Effects of nonequilibrium fluctuations on ultrafast short-range electron transfer dynamics.Nature communications · 2020Article
- Mechanical Unfolding of Single Polyubiquitin Molecules Reveals Evidence of Dynamic Disorder.ACS omega · 2020Article
- Nonequilibrium dynamics of photoinduced forward and backward electron transfer reactions.The Journal of chemical physics · 2020Article
- Understanding Short-Range Electron-Transfer Dynamics in Proteins.The journal of physical chemistry letters · 2019Article
- Short-Range Electron Transfer in Reduced Flavodoxin: Ultrafast Nonequilibrium Dynamics Coupled with Protein Fluctuations.The journal of physical chemistry letters · 2018Article
- 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
- NMR Structures and Dynamics in a Prohead RNA Loop that Binds Metal Ions.The journal of physical chemistry letters · 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
- Dynamics and hydration explain failed functional transformation in dehalogenase design.Nature chemical biology · 2014Article
- Dynamic Determination of Active-Site Reactivity in Semiquinone Photolyase by the Cofactor Photoreduction.The journal of physical chemistry letters · 2014Article
- Direct probing of solvent accessibility and mobility at the binding interface of polymerase (Dpo4)-DNA complex.The journal of physical chemistry. A · 2013Article
- Determining complete electron flow in the cofactor photoreduction of oxidized photolyase.Proceedings of the National Academy of Sciences of the United States of America · 2013Article
- Dynamic determination of the functional state in photolyase and the implication for cryptochrome.Proceedings of the National Academy of Sciences of the United States of America · 2013Article
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Authors and funding
11 authors.
Funding
Abstract
Dynamic solvation at binding and active sites is critical to protein recognition and enzyme catalysis. We report here the complete characterization of ultrafast solvation dynamics at the recognition site of photoantenna molecule and at the active site of cofactor/substrate in enzyme photolyase by examining femtosecond-resolved fluorescence dynamics and the entire emission spectra. With direct use of intrinsic antenna and cofactor chromophores, we observed the local environment relaxation on the time scales from a few picoseconds to nearly a nanosecond. Unlike conventional solvation where the Stokes shift is apparent, we observed obvious spectral shape changes with the minor, small, and large spectral shifts in three function sites. These emission profile changes directly reflect the modulation of chromophore's excited states by locally constrained protein and trapped-water collective motions. Such heterogeneous dynamics continuously tune local configurations to optimize photolyase's function through resonance energy transfer from the antenna to the cofactor for energy efficiency and then electron transfer between the cofactor and the substrate for repair of damaged DNA. Such unusual solvation and synergetic dynamics should be general in function sites of proteins.
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