Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket

doi:10.1103/PhysRevLett.123.187801

Title: Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket

Abstract

The configuration of charged polymers is heavily dependent on interactions with surrounding salt ions, typically manifesting as a sensitivity to the bulk ionic strength. In this work, we use single-molecule mechanical measurements to show that a charged polysaccharide, hyaluronic acid, reflects an interesting regime of insensitivity to ionic strength in the presence of trivalent ions. Using simulations and theory, we propose that this is caused by the formation of a “jacket” of ions, tightly associated with the polymer, whose charge (and thus effect on configuration) is robust against changes in solution composition.

Authors:

^[1]; Pincus, Philip A. ^[1]; Stevens, Mark J. ^[2]; Saleh, Omar A. ^[1]

Univ. of California, Santa Barbara, CA (United States)
Sandia National Laboratories (SNL), Albuquerque, NM, and Livermore, CA (United States)

Publication Date:: 2019-10-29

Research Org.:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)

OSTI Identifier:: 1574458

Report Number(s):: SAND-2019-12489J
Journal ID: ISSN 0031-9007; PRLTAO; 680392

Grant/Contract Number:: AC04-94AL85000; NA-0003525

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Letters

Additional Journal Information:: Journal Volume: 123; Journal Issue: 18; Journal ID: ISSN 0031-9007

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Innes-Gold, Sarah N., Pincus, Philip A., Stevens, Mark J., and Saleh, Omar A. Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket.  United States: N. p., 2019. 
        Web.  doi:10.1103/PhysRevLett.123.187801.

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                    Innes-Gold, Sarah N., Pincus, Philip A., Stevens, Mark J., & Saleh, Omar A. Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket.  United States.  doi:10.1103/PhysRevLett.123.187801.

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                    Innes-Gold, Sarah N., Pincus, Philip A., Stevens, Mark J., and Saleh, Omar A. Tue .  
        "Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket".  United States.  doi:10.1103/PhysRevLett.123.187801.  https://www.osti.gov/servlets/purl/1574458.

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@article{osti_1574458,

  title        = {Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket},

  author       = {Innes-Gold, Sarah N. and Pincus, Philip A. and Stevens, Mark J. and Saleh, Omar A.},

  abstractNote = {The configuration of charged polymers is heavily dependent on interactions with surrounding salt ions, typically manifesting as a sensitivity to the bulk ionic strength. In this work, we use single-molecule mechanical measurements to show that a charged polysaccharide, hyaluronic acid, reflects an interesting regime of insensitivity to ionic strength in the presence of trivalent ions. Using simulations and theory, we propose that this is caused by the formation of a “jacket” of ions, tightly associated with the polymer, whose charge (and thus effect on configuration) is robust against changes in solution composition.},

  doi          = {10.1103/PhysRevLett.123.187801},

  journal      = {Physical Review Letters},

  number       = 18,

  volume       = 123,

  place        = {United States},

  year         = {2019},

  month        = {10}

}

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DOI: 10.1103/PhysRevLett.123.187801

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Similar Records

Title: Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket

Abstract

Citation Formats

Influence of higher valent ions on flexible polyelectrolyte stiffness and counter-ion distribution journal, April 2016

Langevin dynamics simulation of counterion distribution around isolated flexible polyelectrolyte chains journal, June 2002

Competition between condensation of monovalent and multivalent ions in DNA aggregation journal, August 2004

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Counterion associative behavior with flexible polyelectrolytes journal, September 2004

Molecular Mechanism of Specific Ion Interactions between Alkali Cations and Acetate Anion in Aqueous Solution: A Molecular Dynamics Study journal, June 2012

Dependence of DNA Persistence Length on Ionic Strength and Ion Type journal, January 2019

Electrostatic Persistence Length of a Wormlike Polyelectrolyte journal, September 1977

Magnetic Tweezers: Micromanipulation and Force Measurement at the Molecular Level journal, June 2002

Stretching DNA journal, December 1995

Adsorption of Divalent Cations on DNA journal, October 2004

Reversible Adhesion with Polyelectrolyte Brushes Tailored via the Uptake and Release of Trivalent Lanthanum Ions journal, April 2015

Hyaluronan: A simple polysaccharide with diverse biological functions journal, April 2014

EPR Spectroscopic Characterization of Local Nanoscopic Heterogeneities during the Thermal Collapse of Thermoresponsive Dendronized Polymers journal, July 2010

The effect of chain stiffness and salt on the elastic response of a polyelectrolyte journal, October 2018

Experimental approaches to hyaluronan structure journal, April 2005

Ionic effects on the elasticity of single DNA molecules journal, June 1997

Conformation of Poly(styrenesulfonate) Polyions in the Presence of Multivalent Ions: Small-Angle Neutron Scattering Experiments journal, May 2001

Polyelectrolyte properties of sodium hyaluronate. 2. Potentiometric titration of hyaluronic acid journal, March 1982

Electrostatic Effects on the Conformation and Elasticity of Hyaluronic Acid, a Moderately Flexible Polyelectrolyte journal, January 2017

Effect of calcium ions and pH on the morphology and mechanical properties of hyaluronan brushes journal, February 2019

Similarities between polyelectrolyte gels and biopolymer solutions journal, January 2006

Enhanced chemotherapeutic efficacy of the low-dose doxorubicin in breast cancer via nanoparticle delivery system crosslinked hyaluronic acid journal, January 2019

Detailed scaling analysis of low-force polyelectrolyte elasticity journal, October 2009

Extremely Charged and Incredibly Soft: Physical Characterization of the Pericellular Matrix journal, March 2013

Aqueous and solid complexes of iron(III) with hyaluronic acid journal, April 2002

All-Atom MD Simulation of DNA Condensation Using Ab Initio Derived Force Field Parameters of Cobalt(III)-Hexammine journal, August 2017

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Structure and dynamics of condensed multivalent ions within polyelectrolyte bundles: a combined x-ray diffraction and solid-state NMR study journal, March 2005

Multiplexed single-molecule measurements with magnetic tweezers journal, January 2008

Limiting Laws and Counterion Condensation in Polyelectrolyte Solutions I. Colligative Properties journal, August 1969

Power spectrum and Allan variance methods for calibrating single-molecule video-tracking instruments journal, February 2012

Colloid stabilization with grafted polyelectrolytes journal, May 1991

Collapse of Polyelectrolyte Macromolecules by Counterion Condensation and Ion Pair Formation: A Molecular Dynamics Simulation Study journal, April 1998

DNA Bending by Small, Mobile Multivalent Cations journal, June 1998

A Study of Polyelectrolyte Brushes Formed from Adsorption of Amphiphilic Diblock Copolymers Using the Surface Forces Apparatus journal, December 2002

Interactions between Hyaluronan and Its Receptors (CD44, RHAMM) Regulate the Activities of Inflammation and Cancer journal, May 2015

Distribution of counterions around a cylindrical polyelectrolyte and manning's condensation theory journal, February 1984

Distribution of counterions near discretely charged planes and rods journal, April 2004

50th Anniversary Perspective : A Perspective on Polyelectrolyte Solutions journal, December 2017

Influence of higher valent ions on flexible polyelectrolyte stiffness and counter-ion distribution
journal, April 2016

Langevin dynamics simulation of counterion distribution around isolated flexible polyelectrolyte chains
journal, June 2002

Competition between condensation of monovalent and multivalent ions in DNA aggregation
journal, August 2004

Bioreducible Shell-Cross-Linked Hyaluronic Acid Nanoparticles for Tumor-Targeted Drug Delivery
journal, January 2015

Counterion associative behavior with flexible polyelectrolytes
journal, September 2004

Molecular Mechanism of Specific Ion Interactions between Alkali Cations and Acetate Anion in Aqueous Solution: A Molecular Dynamics Study
journal, June 2012

Dependence of DNA Persistence Length on Ionic Strength and Ion Type
journal, January 2019

Electrostatic Persistence Length of a Wormlike Polyelectrolyte
journal, September 1977

Magnetic Tweezers: Micromanipulation and Force Measurement at the Molecular Level
journal, June 2002

Stretching DNA
journal, December 1995

Adsorption of Divalent Cations on DNA
journal, October 2004

Reversible Adhesion with Polyelectrolyte Brushes Tailored via the Uptake and Release of Trivalent Lanthanum Ions
journal, April 2015

Hyaluronan: A simple polysaccharide with diverse biological functions
journal, April 2014

EPR Spectroscopic Characterization of Local Nanoscopic Heterogeneities during the Thermal Collapse of Thermoresponsive Dendronized Polymers
journal, July 2010

The effect of chain stiffness and salt on the elastic response of a polyelectrolyte
journal, October 2018

Experimental approaches to hyaluronan structure
journal, April 2005

Ionic effects on the elasticity of single DNA molecules
journal, June 1997

Conformation of Poly(styrenesulfonate) Polyions in the Presence of Multivalent Ions: Small-Angle Neutron Scattering Experiments
journal, May 2001

Polyelectrolyte properties of sodium hyaluronate. 2. Potentiometric titration of hyaluronic acid
journal, March 1982

Electrostatic Effects on the Conformation and Elasticity of Hyaluronic Acid, a Moderately Flexible Polyelectrolyte
journal, January 2017

Effect of calcium ions and pH on the morphology and mechanical properties of hyaluronan brushes
journal, February 2019

Similarities between polyelectrolyte gels and biopolymer solutions
journal, January 2006

Enhanced chemotherapeutic efficacy of the low-dose doxorubicin in breast cancer via nanoparticle delivery system crosslinked hyaluronic acid
journal, January 2019

Detailed scaling analysis of low-force polyelectrolyte elasticity
journal, October 2009

Extremely Charged and Incredibly Soft: Physical Characterization of the Pericellular Matrix
journal, March 2013

Aqueous and solid complexes of iron(III) with hyaluronic acid
journal, April 2002

All-Atom MD Simulation of DNA Condensation Using Ab Initio Derived Force Field Parameters of Cobalt(III)-Hexammine
journal, August 2017

A high-speed magnetic tweezer beyond 10,000 frames per second
journal, April 2013

A crystallographic study of the binding of 13 metal ions to two related RNA duplexes
journal, May 2003

Salt Species-Dependent Electrostatic Effects on ssDNA Elasticity
journal, April 2011

Structure and dynamics of condensed multivalent ions within polyelectrolyte bundles: a combined x-ray diffraction and solid-state NMR study
journal, March 2005

Multiplexed single-molecule measurements with magnetic tweezers
journal, January 2008

Limiting Laws and Counterion Condensation in Polyelectrolyte Solutions I. Colligative Properties
journal, August 1969

Power spectrum and Allan variance methods for calibrating single-molecule video-tracking instruments
journal, February 2012

Colloid stabilization with grafted polyelectrolytes
journal, May 1991

Collapse of Polyelectrolyte Macromolecules by Counterion Condensation and Ion Pair Formation: A Molecular Dynamics Simulation Study
journal, April 1998

DNA Bending by Small, Mobile Multivalent Cations
journal, June 1998

A Study of Polyelectrolyte Brushes Formed from Adsorption of Amphiphilic Diblock Copolymers Using the Surface Forces Apparatus
journal, December 2002

Interactions between Hyaluronan and Its Receptors (CD44, RHAMM) Regulate the Activities of Inflammation and Cancer
journal, May 2015

Distribution of counterions around a cylindrical polyelectrolyte and manning's condensation theory
journal, February 1984

Distribution of counterions near discretely charged planes and rods
journal, April 2004

50th Anniversary Perspective : A Perspective on Polyelectrolyte Solutions
journal, December 2017