Journal ArticleDOI
Protein Conformational Dynamics Probed by Single-Molecule Electron Transfer
Haw Yang,Haw Yang,Haw Yang,Guobin Luo,Guobin Luo,Guobin Luo,Pallop Karnchanaphanurach,Pallop Karnchanaphanurach,Pallop Karnchanaphanurach,Tai Man Louie,Tai Man Louie,Tai Man Louie,Ivan Rech,Ivan Rech,Ivan Rech,Sergio Cova,Sergio Cova,Sergio Cova,Luying Xun,Luying Xun,Luying Xun,X. Sunney Xie,X. Sunney Xie,X. Sunney Xie +23 more
TLDR
By probing the fluorescence lifetime of the single flavin on a photon-by-photon basis, the variation of flavin-tyrosine distance over time is observed, suggesting the existence of multiple interconverting conformers related to the fluctuating catalytic reactivity.Abstract:
Electron transfer is used as a probe for angstrom-scale structural changes in single protein molecules. In a flavin reductase, the fluorescence of flavin is quenched by a nearby tyrosine residue by means of photo-induced electron transfer. By probing the fluorescence lifetime of the single flavin on a photon-by-photon basis, we were able to observe the variation of flavin-tyrosine distance over time. We could then determine the potential of mean force between the flavin and the tyrosine, and a correlation analysis revealed conformational fluctuation at multiple time scales spanning from hundreds of microseconds to seconds. This phenomenon suggests the existence of multiple interconverting conformers related to the fluctuating catalytic reactivity.read more
Citations
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Journal ArticleDOI
Fluoroacetate dehalogenase catalyzed dehalogenation of halogenated carboxylic acids: A QM/MM approach.
TL;DR: It is proposed that mutation of the binding pocket amino acids to smaller proton donor amino acids may increase the efficiency for dechlorination and debromination, which may of practical value for the efficient degradation of chlorined and bromined pollutants by harnessing FAcD.
Journal ArticleDOI
Flavoprotein Photochemistry: Fundamental Processes and Photocatalytic Perspectives.
TL;DR: This Perspective outlines work on the characterization of early reaction intermediates not only in the relatively well-studied resting oxidized forms but also in the fully reduced and the intrinsically unstable semireduced forms, where ultrafast photooxidation of flavin was recently demonstrated.
Journal ArticleDOI
Foldamers with Hybrid Biological and Synthetic Sequences as Selective DNA Fluorescent Probes
TL;DR: Foldable polymers with alternating single-strand deoxyribonucleic acid (ssDNA) and planar fluorescent organic chromophores can self-organize into folded nanostructures and hence are hybrid foldamers with biological sequences and synthetic properties, which may find important applications as biological probes.
Journal ArticleDOI
Time-resolved fluctuation during the photochemical reaction of a photoreceptor protein: phototropin1LOV2-linker.
Kunisato Kuroi,Francielle Sato,Yusuke Nakasone,Kazunori Zikihara,Satoru Tokutomi,Masahide Terazima +5 more
TL;DR: It is concluded that the cavity volumes between the LOV domain and the linker domain increase in the S state, which explains the enhanced compressibility of the phot1LOV2-linker.
DissertationDOI
Observation of Single-Molecule Rotational Diffusion at Microsecond Timescale by Polarized Fluorescence Correlation Spectroscopy
TL;DR: In this article, the authors present a series of experimental and numerical studies of macromolecular organic, inorganic and biological structures, in all instances focusing on the behavior characteristic of individual discrete molecular elements, and they reach the conclusion that the molecular structure and nanoscale surface interaction potential unique to carbon nanotubes collectively give rise to atomic force microscopy imaging artifacts manifesting as apparent lateral topographic resolution significantly better than that predicted by the probe and sample structures.
References
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Rudolph A. Marcus,Norman Sutin +1 more
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Journal ArticleDOI
Formation of glasses from liquids and biopolymers.
TL;DR: The onset of a sharp change in ddT( is the Debye-Waller factor and T is temperature) in proteins, which is controversially indentified with the glass transition in liquids, is shown to be general for glass formers and observable in computer simulations of strong and fragile ionic liquids, where it proves to be close to the experimental glass transition temperature.
Journal ArticleDOI
The energy landscapes and motions of proteins.
TL;DR: The concepts that emerge from studies of the conformational substates and the motions between them permit a quantitative discussion of one simple reaction, the binding of small ligands such as carbon monoxide to myoglobin.
Journal ArticleDOI
Fluorescence spectroscopy of single biomolecules.
TL;DR: The progress in applying single-molecule detection and single-Molecule spectroscopy at room temperature by laser-induced fluorescence with the use of fluorophores that are site-specifically attached to macromolecules is reviewed.