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Anion hydration is complicated by H-bond donation between neighboring water molecules in addition to H-bond donation to the anion. This situation can lead to competing structures for chemically simple clusters like (H$_2$O)$_n$Cl$^-$ and to…

Chemical Physics · Physics 2021-10-04 A. Muralidharan , L. R. Pratt , M. I. Chaudhari , S. B. Rempe

Accurate predictions of the hydration free energy for anions typically have been more challenging than for cations. Hydrogen bond donation to the anion in hydrated clusters such as $\mathrm{F(H_2O)}_n{}^-$ can lead to delicate structures.…

Chemical Physics · Physics 2019-03-06 A. Muralidharan , L. R. Pratt , M. I. Chaudhari , S. B. Rempe

The interactions of hydrated ions with solution and interface partners are strong on a chemical energy scale. Here, we test the foremost \textit{ab initio theory} for evaluation of hydration free energies of ions, namely,…

Chemical Physics · Physics 2022-06-27 Diego T. Gomez , Lawrence R. Pratt , Dilipkumar N. Asthagiri , Susan B. Rempe

A theoretical study of the structural and electronic properties of the chloride ion and water molecules in the first hydration shell is presented. The calculations are performed on an ensemble of configurations obtained from molecular…

Soft Condensed Matter · Physics 2015-05-14 Zhen Zhao , David M. Rogers , Thomas L. Beck

Within the quasichemical approach, the hydration free energy of an ion is decomposed into a chemical term accounting for ion specific ion-water interactions within the coordination sphere and nonspecific contributions accounting for packing…

Biological Physics · Physics 2011-06-03 Safir Merchant , D. Asthagiri

Quasi-chemical theory applied to ion hydration combines statistical mechanical theory, electronic structure calculations, and molecular simulation, disciplines which are individually subjects for specialized professional attention. Because…

Chemical Physics · Physics 2013-03-14 D. Sabo , D. Jiao , S. Varma , L. R. Pratt , S. B. Rempe

Thermochemistry of gas-phase ion-water clusters together with estimates of the hydration free energy of the clusters and the water ligands are used to calculate the hydration free energy of the ion. Often the hydration calculations use a…

Biological Physics · Physics 2015-05-28 Safir Merchant , Purushottam D. Dixit , Kelsey R. Dean , D. Asthagiri

Treating water as a linearly responding dielectric continuum on molecular length scales allows very simple estimates of solvation structure and thermodynamics for charged and polar solutes. While this approach can successfully account for…

Statistical Mechanics · Physics 2021-07-07 Stephen J. Cox , Kranthi K. Mandadapu , Phillip L. Geissler

The adsorption of anions from aqueous solution on the air/water interface controls important heterogeneous chemistry in the atmosphere and is thought to have similar physics to anion adsorption at hydrophobic interfaces more generally.…

Chemical Physics · Physics 2018-05-09 Yujin Tong , Igor Ying Zhang , R. Kramer Campen

Experimental studies on ion-water clusters have provided insights into the microscopic aspects of hydration phenomena. One common view is that extending those experimental studies to larger cluster sizes would give the single ion absolute…

Chemical Physics · Physics 2009-11-10 D. Asthagiri , Lawrence R. Pratt , H. S. Ashbaugh

The HO$^-$(aq) ion participates in myriad aqueous phase chemical processes of biological and chemical interest. A molecularly valid description of its hydration state, currently poorly understood, is a natural prerequisite to modeling…

Chemical Physics · Physics 2009-11-10 D. Asthagiri , Lawrence R. Pratt , J. D. Kress , M. A. Gomez

The quasi-chemical organization of the potential distribution theorem -- molecular quasi-chemical theory (QCT) -- enables practical calculations and also provides a conceptual framework for molecular hydration phenomena. QCT can be viewed…

Chemical Physics · Physics 2021-05-14 Dilipkumar N. Asthagiri , Michael E. Paulaitis , Lawrence R. Pratt

Non-local electrostatic interactions associated with the finite solvent size and ion polarizability are investigated within the mean-field linear response theory. To this end, we introduce a field theoretic model of a polar liquid composed…

Soft Condensed Matter · Physics 2015-06-15 Sahin Buyukdagli , Tapio Ala-Nissila

This work constructs an advanced force field, the Completely Multipolar Model (CMM), to quantitatively reproduce each term of an energy decomposition analysis (EDA) for aqueous solvated alkali metal cations and halide anions and their ion…

Chemical Physics · Physics 2024-10-14 J. P. Heindel , L. Kim , M. Head-Gordon , T. Head-Gordon

Recent developments in molecular theories and simulation of ions and polar molecules in water are reviewed. The hydration of imidazole and imidazolium solutes is used to exemplify the theoretical issues. The treatment of long-ranged…

Chemical Physics · Physics 2016-09-28 Gerhard Hummer , Lawrence R. Pratt , Angel E. Garcia

We develop a quasi-chemical theory for the study of packing thermodynamics in dense liquids. The situation of hard-core interactions is addressed by considering the binding of solvent molecules to a precisely defined `cavity' in order to…

Chemical Physics · Physics 2007-05-23 Lawrence R. Pratt , Randall A. LaViolette , Maria A. Gomez , Mary E. Gentile

The goal of this work is to propose a simple continuous model that captures the dielectric properties of water at the nanometric scale. We write an electrostatic energy as a functional of the polarisation field containing a term in $P^4$…

Chemical Physics · Physics 2019-04-09 Hélène Berthoumieux , Fabien Paillusson

A statistical thermodynamic development is given of a new implicit solvent model that avoids the traditional system size limitations of computer simulation of macromolecular solutions with periodic boundary conditions. This implicit solvent…

Chemical Physics · Physics 2009-10-31 Lawrence R. Pratt , Susan B. Rempe

We present a Ginzburg-Landau theory of inhomogeneous polyelectrolytes with a polar solvent. First, we take into account the molecular (solvation) interaction among the ions, the charged monomers, the uncharged monomers, and the solvent…

Soft Condensed Matter · Physics 2009-03-10 Akira Onuki , Ryuichi Okamoto

Ion specificity and related Hofmeister effects, ubiquitous in aqueous systems, can have spectacular consequences in hydrated clays, where ion-specific nanoscale surface forces can determine large scale cohesive, swelling and shrinkage…

Soft Condensed Matter · Physics 2022-12-02 Francis Dragulet , Abhay Goyal , Katerina Ioannidou , Roland J. -M. Pellenq , Emanuela Del Gado
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