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Title: Short-Time Glassy Dynamics in Viscous Protein Solutions with Competing Interactions

Abstract

Although there have been numerous investigations of the glass transition for colloidal dispersions with only a short-ranged attraction, less is understood for systems interacting with a long-ranged repulsion in addition to this attraction, which is ubiquitous in aqueous protein solutions at low ionic strength. Highly puri ed concentrated lysozyme solutions are used as a model system and investigated over a large range of protein concentrations at very low ionic strength. Newtonian liquid behavior is observed at all concentrations, even up to 480 mg/mL, where the zero shear viscosity increases by more than three orders of magnitude with increasing concentration. Remarkably, despite this macroscopic liquid-like behavior, the measurements of the dynamics in the short-time limit shows features typical of glassy colloidal systems. Investigation of the inter-protein structure indicates that the reduced short-time mobility of the protein is caused by localized regions of high density within a heterogeneous density distribution. This structural heterogeneity occurs on intermediate range length scale, driven by the competing potential features, and is distinct from commonly studied colloidal gel systems in which a heterogeneous density distribution tends to extend to the whole system. The presence of long-ranged repulsion also allows for more mobility over large length and longmore » time scales resulting in the macroscopic relaxation of the structure. The experimental results provide evidence for the need to explicitly include intermediate range order in theories for the macroscopic properties of protein solutions interacting via competing potential features.« less

Authors:
 [1];  [2];  [3];  [4];  [4];  [1];  [2]
  1. Univ. of Delaware, Newark, DE (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Inst. Laue-Langevin (ILL), Grenoble (France)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1286934
Alternate Identifier(s):
OSTI ID: 1227033
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 115; Journal Issue: 22; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Godfrin, P. Douglas, Hudson, Steven, Hong, Kunlun, Porcar, Lionel, Falus, Peter, Wagner, Norman, and Liu, Yun. Short-Time Glassy Dynamics in Viscous Protein Solutions with Competing Interactions. United States: N. p., 2015. Web. doi:10.1103/PhysRevLett.115.228302.
Godfrin, P. Douglas, Hudson, Steven, Hong, Kunlun, Porcar, Lionel, Falus, Peter, Wagner, Norman, & Liu, Yun. Short-Time Glassy Dynamics in Viscous Protein Solutions with Competing Interactions. United States. https://doi.org/10.1103/PhysRevLett.115.228302
Godfrin, P. Douglas, Hudson, Steven, Hong, Kunlun, Porcar, Lionel, Falus, Peter, Wagner, Norman, and Liu, Yun. 2015. "Short-Time Glassy Dynamics in Viscous Protein Solutions with Competing Interactions". United States. https://doi.org/10.1103/PhysRevLett.115.228302. https://www.osti.gov/servlets/purl/1286934.
@article{osti_1286934,
title = {Short-Time Glassy Dynamics in Viscous Protein Solutions with Competing Interactions},
author = {Godfrin, P. Douglas and Hudson, Steven and Hong, Kunlun and Porcar, Lionel and Falus, Peter and Wagner, Norman and Liu, Yun},
abstractNote = {Although there have been numerous investigations of the glass transition for colloidal dispersions with only a short-ranged attraction, less is understood for systems interacting with a long-ranged repulsion in addition to this attraction, which is ubiquitous in aqueous protein solutions at low ionic strength. Highly puri ed concentrated lysozyme solutions are used as a model system and investigated over a large range of protein concentrations at very low ionic strength. Newtonian liquid behavior is observed at all concentrations, even up to 480 mg/mL, where the zero shear viscosity increases by more than three orders of magnitude with increasing concentration. Remarkably, despite this macroscopic liquid-like behavior, the measurements of the dynamics in the short-time limit shows features typical of glassy colloidal systems. Investigation of the inter-protein structure indicates that the reduced short-time mobility of the protein is caused by localized regions of high density within a heterogeneous density distribution. This structural heterogeneity occurs on intermediate range length scale, driven by the competing potential features, and is distinct from commonly studied colloidal gel systems in which a heterogeneous density distribution tends to extend to the whole system. The presence of long-ranged repulsion also allows for more mobility over large length and long time scales resulting in the macroscopic relaxation of the structure. The experimental results provide evidence for the need to explicitly include intermediate range order in theories for the macroscopic properties of protein solutions interacting via competing potential features.},
doi = {10.1103/PhysRevLett.115.228302},
url = {https://www.osti.gov/biblio/1286934}, journal = {Physical Review Letters},
issn = {0031-9007},
number = 22,
volume = 115,
place = {United States},
year = {Tue Nov 24 00:00:00 EST 2015},
month = {Tue Nov 24 00:00:00 EST 2015}
}

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Cited by: 55 works
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Works referencing / citing this record:

Short-time dynamics of lysozyme solutions with competing short-range attraction and long-range repulsion: Experiment and theory
journal, February 2018


Multi-attribute PAT for UF/DF of Proteins—Monitoring Concentration, particle sizes, and Buffer Exchange
journal, February 2020


Dynamic cluster formation determines viscosity and diffusion in dense protein solutions
journal, April 2019


Recovery, overloading, and protein interactions in asymmetrical flow field-flow fractionation
journal, February 2019


Dynamics of proteins in solution
journal, January 2019


Microliter viscometry using a bright-field microscope: η -DDM
journal, January 2018


Tween protects recombinant human growth hormone against agitation-induced damage via hydrophobic interactions
journal, December 1998