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
Stretched exponential decay and correlations in the catalytic activity of fluctuating single lipase molecules
Ophir Flomenbom,Kelly Velonia,Davey Loos,Sadahiro Masuo,Mircea Cotlet,Yves Engelborghs,Johan Hofkens,Alan E. Rowan,Roeland J. M. Nolte,Mark Van der Auweraer,Frans C. De Schryver,Joseph Klafter +11 more
TL;DR: The direct observation of a single lipase-catalyzed reaction for extended periods of time (hours) by using confocal fluorescence microscopy implies that the fluctuating enzyme model, which involves a spectrum of enzymatic conformations that interconvert on the time scale of the catalytic activity, best describes the observed enzyme activity.
Journal ArticleDOI
Illuminating the mechanistic roles of enzyme conformational dynamics
Jeffrey A. Hanson,Karl E. Duderstadt,Lucas P. Watkins,Sucharita Bhattacharyya,Jason Brokaw,Jhih-Wei Chu,Haw Yang +6 more
TL;DR: Using the method of high-resolution single-molecule FRET, this analysis shows unambiguously that adenylate kinase is capable of dynamically sampling two distinct states, which correlate well with those observed by x-ray crystallography.
Journal ArticleDOI
Energy dissipation in multichromophoric single dendrimers
TL;DR: In dendrimers with multiple chromophores, energy hopping and transfer to the chromophore with the energetically lowest S(1) state was observed, and the rate constants of forward and backward electron transfer were established.
Journal ArticleDOI
Existence of mild solution for evolution equation with Hilfer fractional derivative
Haibo Gu,Juan J. Trujillo +1 more
TL;DR: By noncompact measure method, some sufficient conditions are obtained to ensure the existence of mild solution of evolution equation with Hilfer fractional derivative which generalized the famous Riemann-Liouville fractional derivatives.
Journal ArticleDOI
A fluorescence light-up Ag nanocluster probe that discriminates single-nucleotide variants by emission color.
TL;DR: This SNP detection method has been validated on all single-nucleotide substitution scenarios in three synthetic DNA targets, in six disease-related SNP targets, and in two clinical samples taken from patients with ovarian serous borderline tumors, making this method a reliable and low-cost assay with a simple readout format.
References
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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.
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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
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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.