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
Single-molecule photoredox catalysis
TL;DR: Photocatalytic dehalogenation by a common dyestuff under aqueous conditions is driven by energy-additive absorption of two photons on the single-molecule level.
Journal ArticleDOI
Two-state analysis of single-molecule Raman spectra of crystal violet
TL;DR: In this article, surface-enhanced Raman spectra of individual crystal violet molecules adsorbed on silver colloids were measured and analyzed, and statistical analysis showed that the dynamic process underlying the spectral jumps is likely to be Markovian.
Journal ArticleDOI
α-Helix C-Terminus Acting as a Relay to Mediate Long-Range Hole Migration in Proteins
Xiaohua Chen,Laibin Zhang,Lei Zhang,Wenming Sun,Zhenwei Zhang,Haiying Liu,Yuxiang Bu,Robert I. Cukier +7 more
TL;DR: In this article, the relay ability of an α-helical C-terminus varies with helix length, capping, proximal group competition, and helix twisting/bending.
Journal ArticleDOI
Single Molecule Conformational Memory Extraction: P5ab RNA Hairpin
Steve Pressé,Jack Peterson,Julian Lee,Phillip Elms,Justin L. MacCallum,Susan Marqusee,Carlos Bustamante,Ken A. Dill +7 more
TL;DR: In this article, the authors show that it is unnecessary to assume either (i) or (ii) and focus their analysis on the zipping/unzipping transitions of an RNA hairpin.
Journal ArticleDOI
Fluorescence quenching induced by conformational fluctuations in unsolvated polypeptides.
TL;DR: The fluorescence lifetime provides a local probe of conformational fluctuations averaged over the ion ensemble, which is consistent with increased fluorescence quenching with temperature resulting from the occurrence of conformers having specific positions of the dye, Trp, and Arg (+).
References
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Journal ArticleDOI
Electron transfers in chemistry and biology
Rudolph A. Marcus,Norman Sutin +1 more
TL;DR: In this paper, the electron transfer reactions between ions and molecules in solution have been the subject of considerable experimental study during the past three decades, including charge transfer, photoelectric emission spectra, chemiluminescent electron transfer, and electron transfer through frozen media.
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.