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Title: Dynamic properties of different liquid states in systems with competing interactions studied with lysozyme solutions

Recent studies of colloidal systems with a short-range attraction and long-range repulsion (SALR) have been demonstrated to have a generalized phase diagram with multiple liquid states defined by their structures. In this paper, we identify the different liquid states of previous experimentally studied lysozyme samples within this proposed generalized state diagram and explore the dynamic properties of each liquid state. We show that most lysozyme samples studied here and previously at low and intermediate concentrations are dispersed fluids while a few high concentration samples are randomly percolated liquids. In the dispersed fluid region, the short-time diffusion coefficient measured by neutron spin echo agrees well with the long time diffusion coefficient estimated with the solution viscosity. This dynamic feature is maintained even for some samples in the random percolated region. However, the short-time and long-time diffusion coefficients of random percolated fluids deviate at larger concentration and attraction strength. At high enough concentrations, the mean square displacement can be as slow as those of many glassy colloidal systems at time scales near the characteristic diffusion time even though these lysozyme samples remain in liquid states at the long-time limit. Here, we thus identify the region in the generalized phase diagram where thesemore » equilibrium states with extremely slow local dynamics exist relative to bulk percolation and kinetic arrest (gel and glassy) transitions.« less
Authors:
ORCiD logo [1] ;  [2] ;  [2] ; ORCiD logo [3] ;  [4] ;  [5] ;  [6]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Univ. of Delaware, Newark, DE (United States)
  2. Institut Laue-Langevin, Grenoble Cedex (France)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  5. Univ. of Delaware, Newark, DE (United States)
  6. Univ. of Delaware, Newark, DE (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Soft Matter
Additional Journal Information:
Journal Volume: 14; Journal Issue: 42; Journal ID: ISSN 1744-683X
Publisher:
Royal Society of Chemistry
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1480635

Godfrin, P. Douglas, Falus, Peter, Porcar, Lionel, Hong, Kunlun, Hudson, Steven D., Wagner, Norman J., and Liu, Yun. Dynamic properties of different liquid states in systems with competing interactions studied with lysozyme solutions. United States: N. p., Web. doi:10.1039/C8SM01678J.
Godfrin, P. Douglas, Falus, Peter, Porcar, Lionel, Hong, Kunlun, Hudson, Steven D., Wagner, Norman J., & Liu, Yun. Dynamic properties of different liquid states in systems with competing interactions studied with lysozyme solutions. United States. doi:10.1039/C8SM01678J.
Godfrin, P. Douglas, Falus, Peter, Porcar, Lionel, Hong, Kunlun, Hudson, Steven D., Wagner, Norman J., and Liu, Yun. 2018. "Dynamic properties of different liquid states in systems with competing interactions studied with lysozyme solutions". United States. doi:10.1039/C8SM01678J. https://www.osti.gov/servlets/purl/1480635.
@article{osti_1480635,
title = {Dynamic properties of different liquid states in systems with competing interactions studied with lysozyme solutions},
author = {Godfrin, P. Douglas and Falus, Peter and Porcar, Lionel and Hong, Kunlun and Hudson, Steven D. and Wagner, Norman J. and Liu, Yun},
abstractNote = {Recent studies of colloidal systems with a short-range attraction and long-range repulsion (SALR) have been demonstrated to have a generalized phase diagram with multiple liquid states defined by their structures. In this paper, we identify the different liquid states of previous experimentally studied lysozyme samples within this proposed generalized state diagram and explore the dynamic properties of each liquid state. We show that most lysozyme samples studied here and previously at low and intermediate concentrations are dispersed fluids while a few high concentration samples are randomly percolated liquids. In the dispersed fluid region, the short-time diffusion coefficient measured by neutron spin echo agrees well with the long time diffusion coefficient estimated with the solution viscosity. This dynamic feature is maintained even for some samples in the random percolated region. However, the short-time and long-time diffusion coefficients of random percolated fluids deviate at larger concentration and attraction strength. At high enough concentrations, the mean square displacement can be as slow as those of many glassy colloidal systems at time scales near the characteristic diffusion time even though these lysozyme samples remain in liquid states at the long-time limit. Here, we thus identify the region in the generalized phase diagram where these equilibrium states with extremely slow local dynamics exist relative to bulk percolation and kinetic arrest (gel and glassy) transitions.},
doi = {10.1039/C8SM01678J},
journal = {Soft Matter},
number = 42,
volume = 14,
place = {United States},
year = {2018},
month = {10}
}

Works referenced in this record:

Reduction and analysis of SANS and USANS data using IGOR Pro
journal, November 2006

Phase Behavior of Small Attractive Colloidal Particles
journal, January 1996
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  • Physical Review Letters, Vol. 76, Issue 1, p. 150-153
  • DOI: 10.1103/PhysRevLett.76.150