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Title: The effect of chain stiffness and salt on the elastic response of a polyelectrolyte

Here, We present simulations of the force-extension curves of strong polyelectrolytes with varying intrinsic stiffness as well as specifically treating hyaluronic acid, a polyelectrolyte of intermediate stiffness. Whereas fully flexible polyelectrolytes show a high-force regime where extension increases nearly logarithmically with force, we find that the addition of even a small amount of stiffness alters the short-range structure and removes this logarithmic elastic regime. This further confirms that the logarithmic regime is a consequence of the short-ranged “wrinkles” in the flexible chain. As the stiffness increases, the force-extension curves tend toward and reach the wormlike chain behavior. Using the screened Coulomb potential and a simple bead-spring model, the simulations are able to reproduce the hyaluronic acid experimental force-extension curves for salt concentrations ranging from 1 to 500 mM. Furthermore, the simulation data can be scaled to a universal curve like the experimental data. The scaling analysis is consistent with the interpretation that, in the low-salt limit, the hyaluronic acid chain stiffness scales with salt with an exponent of –0.7, rather than either of the two main theoretical predictions of –0.5 and –1. Furthermore, given the conditions of the simulation, we conclude that this exponent value is not due to counterionmore » condensation effects, as had previously been suggested.« less
Authors:
 [1] ;  [2] ; ORCiD logo [3]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. Univ. of California, Santa Barbara, CA (United States); Brandeis Univ., Waltham, MA (United States)
  3. Univ. of California, Santa Barbara, CA (United States)
Publication Date:
Report Number(s):
SAND-2018-9832J
Journal ID: ISSN 0021-9606; 667684
Grant/Contract Number:
AC04-94AL85000; NA0003525
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 149; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1473953
Alternate Identifier(s):
OSTI ID: 1461567

Stevens, Mark J., Berezney, John P., and Saleh, Omar A.. The effect of chain stiffness and salt on the elastic response of a polyelectrolyte. United States: N. p., Web. doi:10.1063/1.5035340.
Stevens, Mark J., Berezney, John P., & Saleh, Omar A.. The effect of chain stiffness and salt on the elastic response of a polyelectrolyte. United States. doi:10.1063/1.5035340.
Stevens, Mark J., Berezney, John P., and Saleh, Omar A.. 2018. "The effect of chain stiffness and salt on the elastic response of a polyelectrolyte". United States. doi:10.1063/1.5035340.
@article{osti_1473953,
title = {The effect of chain stiffness and salt on the elastic response of a polyelectrolyte},
author = {Stevens, Mark J. and Berezney, John P. and Saleh, Omar A.},
abstractNote = {Here, We present simulations of the force-extension curves of strong polyelectrolytes with varying intrinsic stiffness as well as specifically treating hyaluronic acid, a polyelectrolyte of intermediate stiffness. Whereas fully flexible polyelectrolytes show a high-force regime where extension increases nearly logarithmically with force, we find that the addition of even a small amount of stiffness alters the short-range structure and removes this logarithmic elastic regime. This further confirms that the logarithmic regime is a consequence of the short-ranged “wrinkles” in the flexible chain. As the stiffness increases, the force-extension curves tend toward and reach the wormlike chain behavior. Using the screened Coulomb potential and a simple bead-spring model, the simulations are able to reproduce the hyaluronic acid experimental force-extension curves for salt concentrations ranging from 1 to 500 mM. Furthermore, the simulation data can be scaled to a universal curve like the experimental data. The scaling analysis is consistent with the interpretation that, in the low-salt limit, the hyaluronic acid chain stiffness scales with salt with an exponent of –0.7, rather than either of the two main theoretical predictions of –0.5 and –1. Furthermore, given the conditions of the simulation, we conclude that this exponent value is not due to counterion condensation effects, as had previously been suggested.},
doi = {10.1063/1.5035340},
journal = {Journal of Chemical Physics},
number = 16,
volume = 149,
place = {United States},
year = {2018},
month = {7}
}