Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket

Innes-Gold, Sarah N.; Pincus, Philip A.; Stevens, Mark J.; Saleh, Omar A.

doi:10.1103/PhysRevLett.123.187801

Polyelectrolyte Conformation Controlled by a Trivalent-Rich Ion Jacket

Journal Article · Tue Oct 29 00:00:00 EDT 2019 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.123.187801· OSTI ID:1574458

^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

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

Grant/Contract Number:: AC04-94AL85000; NA0003525

OSTI ID:: 1574458

Report Number(s):: SAND--2019-12489J; 680392

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 18 Vol. 123; ISSN 0031-9007; ISSN PRLTAO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (45)

EPR Spectroscopic Characterization of Local Nanoscopic Heterogeneities during the Thermal Collapse of Thermoresponsive Dendronized Polymers Junk, Matthias J. N.; Li, Wen; Schlüter, A. Dieter Angewandte Chemie International Edition, Vol. 49, Issue 33 https://doi.org/10.1002/anie.201001469	journal	July 2010
Distribution of counterions around a cylindrical polyelectrolyte and manning's condensation theory Bret, Marc Le; Zimm, Bruno H. Biopolymers, Vol. 23, Issue 2 https://doi.org/10.1002/bip.360230209	journal	February 1984
Similarities between polyelectrolyte gels and biopolymer solutions Horkay, Ferenc; Hecht, Anne-Marie; Geissler, Erik Journal of Polymer Science Part B: Polymer Physics, Vol. 44, Issue 24 https://doi.org/10.1002/polb.21008	journal	January 2006
Magnetic Tweezers: Micromanipulation and Force Measurement at the Molecular Level Gosse, Charlie; Croquette, Vincent Biophysical Journal, Vol. 82, Issue 6 https://doi.org/10.1016/S0006-3495(02)75672-5	journal	June 2002
DNA Bending by Small, Mobile Multivalent Cations Rouzina, Ioulia; Bloomfield, Victor A. Biophysical Journal, Vol. 74, Issue 6 https://doi.org/10.1016/S0006-3495(98)78021-X	journal	June 1998
Aqueous and solid complexes of iron(III) with hyaluronic acid Mercê, Ana Lucia Ramalho; Marques Carrera, Luiz Carlos; Santos Romanholi, Lilian Kelly Journal of Inorganic Biochemistry, Vol. 89, Issue 3-4 https://doi.org/10.1016/S0162-0134(01)00422-6	journal	April 2002
Hyaluronan: A simple polysaccharide with diverse biological functions Dicker, Kevin T.; Gurski, Lisa A.; Pradhan-Bhatt, Swati Acta Biomaterialia, Vol. 10, Issue 4 https://doi.org/10.1016/j.actbio.2013.12.019	journal	April 2014
Extremely Charged and Incredibly Soft: Physical Characterization of the Pericellular Matrix van Oosten, Anne S.; Janmey, Paul A. Biophysical Journal, Vol. 104, Issue 5 https://doi.org/10.1016/j.bpj.2013.01.035	journal	March 2013
Experimental approaches to hyaluronan structure Cowman, Mary K.; Matsuoka, Shiro Carbohydrate Research, Vol. 340, Issue 5 https://doi.org/10.1016/j.carres.2005.01.022	journal	April 2005
Competition between condensation of monovalent and multivalent ions in DNA aggregation Burak, Yoram; Ariel, Gil; Andelman, David Current Opinion in Colloid & Interface Science, Vol. 9, Issue 1-2 https://doi.org/10.1016/j.cocis.2004.05.002	journal	August 2004
All-Atom MD Simulation of DNA Condensation Using Ab Initio Derived Force Field Parameters of Cobalt(III)-Hexammine Sun, Tiedong; Mirzoev, Alexander; Korolev, Nikolay The Journal of Physical Chemistry B, Vol. 121, Issue 33 https://doi.org/10.1021/acs.jpcb.7b03793	journal	August 2017
Reversible Adhesion with Polyelectrolyte Brushes Tailored via the Uptake and Release of Trivalent Lanthanum Ions Farina, Robert; Laugel, Nicolas; Yu, Jing The Journal of Physical Chemistry C, Vol. 119, Issue 26 https://doi.org/10.1021/acs.jpcc.5b02121	journal	April 2015
Electrostatic Effects on the Conformation and Elasticity of Hyaluronic Acid, a Moderately Flexible Polyelectrolyte Berezney, John P.; Saleh, Omar A. Macromolecules, Vol. 50, Issue 3 https://doi.org/10.1021/acs.macromol.6b02166	journal	January 2017
50th Anniversary Perspective : A Perspective on Polyelectrolyte Solutions Muthukumar, M. Macromolecules, Vol. 50, Issue 24 https://doi.org/10.1021/acs.macromol.7b01929	journal	December 2017
Bioreducible Shell-Cross-Linked Hyaluronic Acid Nanoparticles for Tumor-Targeted Drug Delivery Han, Hwa Seung; Thambi, Thavasyappan; Choi, Ki Young Biomacromolecules, Vol. 16, Issue 2 https://doi.org/10.1021/bm5017755	journal	January 2015
Molecular Mechanism of Specific Ion Interactions between Alkali Cations and Acetate Anion in Aqueous Solution: A Molecular Dynamics Study Annapureddy, Harsha V. R.; Dang, Liem X. The Journal of Physical Chemistry B, Vol. 116, Issue 25 https://doi.org/10.1021/jp301859z	journal	June 2012
Colloid stabilization with grafted polyelectrolytes Pincus, Philip Macromolecules, Vol. 24, Issue 10 https://doi.org/10.1021/ma00010a043	journal	May 1991
Conformation of Poly(styrenesulfonate) Polyions in the Presence of Multivalent Ions: Small-Angle Neutron Scattering Experiments Dubois, E.; Boué, F. Macromolecules, Vol. 34, Issue 11 https://doi.org/10.1021/ma000956u	journal	May 2001
Stretching DNA Marko, John F.; Siggia, Eric D. Macromolecules, Vol. 28, Issue 26 https://doi.org/10.1021/ma00130a008	journal	December 1995
Polyelectrolyte properties of sodium hyaluronate. 2. Potentiometric titration of hyaluronic acid Cleland, Robert L.; Wang, John L.; Detweiler, David M. Macromolecules, Vol. 15, Issue 2 https://doi.org/10.1021/ma00230a037	journal	March 1982
A Study of Polyelectrolyte Brushes Formed from Adsorption of Amphiphilic Diblock Copolymers Using the Surface Forces Apparatus Balastre, Marc; Li, Feng; Schorr, Phillip Macromolecules, Vol. 35, Issue 25 https://doi.org/10.1021/ma011875g	journal	December 2002
Salt Species-Dependent Electrostatic Effects on ssDNA Elasticity McIntosh, D. B.; Saleh, O. A. Macromolecules, Vol. 44, Issue 7 https://doi.org/10.1021/ma1028196	journal	April 2011
Electrostatic Persistence Length of a Wormlike Polyelectrolyte Skolnick, Jeffrey; Fixman, Marshall Macromolecules, Vol. 10, Issue 5 https://doi.org/10.1021/ma60059a011	journal	September 1977
Langevin dynamics simulation of counterion distribution around isolated flexible polyelectrolyte chains Liu, S.; Muthukumar, M. The Journal of Chemical Physics, Vol. 116, Issue 22 https://doi.org/10.1063/1.1476930	journal	June 2002
Limiting Laws and Counterion Condensation in Polyelectrolyte Solutions I. Colligative Properties Manning, Gerald S. The Journal of Chemical Physics, Vol. 51, Issue 3 https://doi.org/10.1063/1.1672157	journal	August 1969
Counterion associative behavior with flexible polyelectrolytes Prabhu, Vivek M.; Amis, Eric J.; Bossev, Dobrin P. The Journal of Chemical Physics, Vol. 121, Issue 9 https://doi.org/10.1063/1.1776556	journal	September 2004
Multiplexed single-molecule measurements with magnetic tweezers Ribeck, Noah; Saleh, Omar A. Review of Scientific Instruments, Vol. 79, Issue 9 https://doi.org/10.1063/1.2981687	journal	January 2008
Power spectrum and Allan variance methods for calibrating single-molecule video-tracking instruments Lansdorp, Bob M.; Saleh, Omar A. Review of Scientific Instruments, Vol. 83, Issue 2 https://doi.org/10.1063/1.3687431	journal	February 2012
A high-speed magnetic tweezer beyond 10,000 frames per second Lansdorp, Bob M.; Tabrizi, Shawn J.; Dittmore, Andrew Review of Scientific Instruments, Vol. 84, Issue 4 https://doi.org/10.1063/1.4802678	journal	April 2013
Influence of higher valent ions on flexible polyelectrolyte stiffness and counter-ion distribution Chremos, Alexandros; Douglas, Jack F. The Journal of Chemical Physics, Vol. 144, Issue 16 https://doi.org/10.1063/1.4947221	journal	April 2016
The effect of chain stiffness and salt on the elastic response of a polyelectrolyte Stevens, Mark J.; Berezney, John P.; Saleh, Omar A. The Journal of Chemical Physics, Vol. 149, Issue 16 https://doi.org/10.1063/1.5035340	journal	October 2018
Ionic effects on the elasticity of single DNA molecules Baumann, C. G.; Smith, S. B.; Bloomfield, V. A. Proceedings of the National Academy of Sciences, Vol. 94, Issue 12 https://doi.org/10.1073/pnas.94.12.6185	journal	June 1997
Enhanced chemotherapeutic efficacy of the low-dose doxorubicin in breast cancer via nanoparticle delivery system crosslinked hyaluronic acid Wang, Qin; Zhong, Yinan; Liu, Wenting Drug Delivery, Vol. 26, Issue 1 https://doi.org/10.1080/10717544.2018.1507057	journal	January 2019
Structure and dynamics of condensed multivalent ions within polyelectrolyte bundles: a combined x-ray diffraction and solid-state NMR study Angelini, Thomas E.; Sanders, Lori K.; Liang, Hongjun Journal of Physics: Condensed Matter, Vol. 17, Issue 14 https://doi.org/10.1088/0953-8984/17/14/001	journal	March 2005
A crystallographic study of the binding of 13 metal ions to two related RNA duplexes Ennifar, E. Nucleic Acids Research, Vol. 31, Issue 10 https://doi.org/10.1093/nar/gkg350	journal	May 2003
Effect of calcium ions and pH on the morphology and mechanical properties of hyaluronan brushes Chen, Xinyue; Richter, Ralf P. Interface Focus, Vol. 9, Issue 2 https://doi.org/10.1098/rsfs.2018.0061	journal	February 2019
Detailed scaling analysis of low-force polyelectrolyte elasticity McIntosh, D. B.; Ribeck, N.; Saleh, O. A. Physical Review E, Vol. 80, Issue 4 https://doi.org/10.1103/PhysRevE.80.041803	journal	October 2009
Dependence of DNA Persistence Length on Ionic Strength and Ion Type Guilbaud, Sébastien; Salomé, Laurence; Destainville, Nicolas Physical Review Letters, Vol. 122, Issue 2 https://doi.org/10.1103/PhysRevLett.122.028102	journal	January 2019
Collapse of Polyelectrolyte Macromolecules by Counterion Condensation and Ion Pair Formation: A Molecular Dynamics Simulation Study Winkler, Roland G.; Gold, Michael; Reineker, Peter Physical Review Letters, Vol. 80, Issue 17 https://doi.org/10.1103/PhysRevLett.80.3731	journal	April 1998
Distribution of counterions near discretely charged planes and rods Henle, M. L.; Santangelo, C. D.; Patel, D. M. Europhysics Letters (EPL), Vol. 66, Issue 2 https://doi.org/10.1209/epl/i2003-10205-1	journal	April 2004
Adsorption of Divalent Cations on DNA Morfin, Isabelle; Horkay, Ferenc; Basser, Peter J. Biophysical Journal, Vol. 87, Issue 4 https://doi.org/10.1529/biophysj.104.045542	journal	October 2004
Interactions between Hyaluronan and Its Receptors (CD44, RHAMM) Regulate the Activities of Inflammation and Cancer Misra, Suniti; Hascall, Vincent C.; Markwald, Roger R. Frontiers in Immunology, Vol. 6 https://doi.org/10.3389/fimmu.2015.00201	journal	May 2015
Dependence of DNA persistence length on ionic strength and ion type Guilbaud, Sébastien; Salomé, Laurence; Destainville, Nicolas arXiv https://doi.org/10.48550/arxiv.1810.01611	text	January 2018
Distribution of counterions near discretely charged planes and rods Henle, Mark L.; Santangelo, Christian D.; Patel, Deena M. arXiv https://doi.org/10.48550/arxiv.cond-mat/0310540	text	January 2003
Competition between condensation of monovalent and multivalent ions in DNA aggregation Burak, Yoram; Ariel, Gil; Andelman, David arXiv https://doi.org/10.48550/arxiv.cond-mat/0407344	text	January 2004

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