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Journal ArticleDOI

Protein Conformational Dynamics Probed by Single-Molecule Electron Transfer

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.

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Citations
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Journal ArticleDOI

Dynamic Disorder in Quasi-Equilibrium Enzymatic Systems

TL;DR: This paper investigates the applicability of macroscopic rate laws for fluctuating enzyme systems in which catalytic transitions are slower than ligand binding-dissociation reactions and shows that the catalytic rate has the same dependence on ligand concentrations as obtained from mass-action kinetics even in the presence of slow conformational fluctuations.
Proceedings ArticleDOI

High-detection efficiency and picosecond timing compact detector modules with red-enhanced SPADs

TL;DR: In this paper, the authors present a compact photon counting and timing module that fills the gap between the high temporal resolution and the high detection efficiency systems, achieving a photon detection efficiency of 37% at 800 nm (peak of 58% at 600 nm) while maintaining a temporal resolution of about 100 ps FWHM.
Journal ArticleDOI

Single-Molecule Monitoring of the Structural Switching Dynamics of Nucleic Acids through Controlling Fluorescence Blinking

TL;DR: A method for kinetic analysis based on control of fluorescence blinking (KACB), a general approach to investigate the dynamics of biomolecules by using a single fluorophore, enabling real‐time single‐molecule measurement of the structure‐changing dynamics of nucleic acids.
Journal ArticleDOI

Ensemble-based characterization of unbound and bound states on protein energy landscape.

TL;DR: In this paper, an analysis of the unbound-to-bound changes points to conformational selection as the binding mechanism for four proteins and showed that bound and unbound spectra often significantly overlap.
References
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疟原虫var基因转换速率变化导致抗原变异[英]/Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A

宁北芳, +1 more
TL;DR: PfPMP1)与感染红细胞、树突状组胞以及胎盘的单个或多个受体作用,在黏附及免疫逃避中起关键的作�ly.
Journal ArticleDOI

Electron transfers in chemistry and biology

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.
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