@article{b4990b736e1444dea7c1cd4be25105a1,
title = "Ion-dependent protein–surface interactions from intrinsic solvent response",
abstract = "The phyllosilicate mineral muscovite mica is widely used as a surface template for the patterning of macromolecules, yet a molecular understanding of its surface chemistry under varying solution conditions, required to predict and control the self-assembly of adsorbed species, is lacking. We utilize all-atom molecular dynamics simulations in conjunction with an electrostatic analysis based in local molecular field theory that affords a clean separation of long-range and short-range electrostatics. Using water polarization response as a measure of the electric fields that arise from patterned, surface-bound ions that direct the adsorption of charged macromolecules, we apply a Landau theory of forces induced by asymmetrically polarized surfaces to compute protein–surface interactions for two muscovite-binding proteins (DHR10-mica6 and C98RhuA). Comparison of the pressure between surface and protein in high-concentration KCl and NaCl aqueous solutions reveals ion-specific differences in far-field protein–surface interactions, neatly capturing the ability of ions to modulate the surface charge of muscovite that in turn selectively attracts one binding face of each protein over all others.",
keywords = "Electrostatics, Landau theory, Soft matter, Solution assembly, Specific ion effects",
author = "Prelesnik, {Jesse L.} and Alberstein, {Robert G.} and Shuai Zhang and Harley Pyles and David Baker and Jim Pfaendtner and {de Yoreo}, {James J.} and Tezcan, {F. Akif} and Remsing, {Richard C.} and Mundy, {Christopher J.}",
note = "Funding Information: ACKNOWLEDGMENTS. The AFM experiments were done in Pacific North-west National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated for the Department of Energy by Battelle under Contract DE-AC05-76RL01830. We thank Sebastien Kerisit for providing simulation data for comparative purposes. We acknowledge helpful conversations with Greg Schenter, Jaehun Chun, Lilo Pozzo, Andy Ferguson, Xin Qi, Mingfei Zhao, Sarah Alamdari, Janani Sampath, and Orion Dollar. This work was Funding Information: The AFM experiments were done in Pacific Northwest National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated for the Department of Energy by Battelle under Contract DE-AC05-76RL01830. We thank Sebastien Kerisit for providing simulation data for comparative purposes. We acknowledge helpful conversations with Greg Schenter, Jaehun Chun, Lilo Pozzo, Andy Ferguson, Xin Qi, Mingfei Zhao, Sarah Alamdari, Janani Sampath, and Orion Dollar. This work was facilitated through the use of advanced computational, storage, and networking infrastructure provided by the Hyak supercomputer system at the University of Washington. This material is based on work supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, as part of the Energy Frontier Research Center program, the Center for the Science of Synthesis Across Scales under Award DE-SC0019288. Funding Information: US Department of Energy, Office of Science, Office of Basic Energy Sciences, as part of the Energy Frontier Research Center program, the Center for the Science of Synthesis Across Scales under Award DE-SC0019288. Publisher Copyright: {\textcopyright} 2021 National Academy of Sciences. All rights reserved.",
year = "2021",
month = jun,
day = "29",
doi = "10.1073/pnas.2025121118",
language = "English (US)",
volume = "118",
journal = "Proceedings of the National Academy of Sciences of the United States of America",
issn = "0027-8424",
publisher = "National Academy of Sciences",
number = "26",
}