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A mixture of solvent particles with short-range, directional interactions and solute particles with short-range, isotropic interactions that can bond multiple times is of fundamental interest in understanding liquids and colloidal mixtures.…

软凝聚态物质 · 物理学 2016-09-21 Artee Bansal , D. Asthagiri , Kenneth R. Cox , Walter G. Chapman

We present a theory to predict the structure and thermodynamics of mixtures of colloids of different diameters, building on our earlier work [J. Chem. Phys. 145, 074904 (2016)] that considered mixtures with all particles constrained to have…

软凝聚态物质 · 物理学 2017-05-24 Artee Bansal , Arjun Valiya Parambathu , D. Asthagiri , Kenneth R. Cox , Walter G. Chapman

We derive an expression for the chemical potential of an associating solute in a solvent relative to the value in a reference fluid using the quasichemical organization of the potential distribution theorem. The fraction of times the solute…

软凝聚态物质 · 物理学 2017-10-25 Artee Bansal , Walter G. Chapman , D. Asthagiri

We are concerned with few-particle correlations in a fermionic system at finite temperature and density. Within the many-body Green functions formalism the description of correlations is provided by the Dyson equation approach that leads to…

核理论 · 物理学 2007-05-23 S. A. Sofianos , M. Beyer

In a recent letter we presented a framework for predicting the concentrations of many-particle local structures inside the bulk liquid as a route to assessing changes in the liquid approaching dynamical arrest. Central to this framework was…

统计力学 · 物理学 2019-12-25 Joshua F. Robinson , Francesco Turci , Roland Roth , C. Paddy Royall

We analyze the slow, glassy structural relaxation as measured through collective and tagged-particle density correlation functions obtained from Brownian dynamics simulations for a polydisperse system of quasi-hard spheres in the framework…

软凝聚态物质 · 物理学 2010-10-18 F. Weysser , A. M. Puertas , M. Fuchs , Th. Voigtmann

Solvation effect might have a tremendous influence on chemical reactions. However, precise quantum chemistry calculations are most often done either in vacuum neglecting the role of the solvent or using continuum solvent model ignoring its…

化学物理 · 物理学 2020-07-14 Guillaume Jeanmairet , Maximilien Levesque , Daniel Borgis

The predictions of the mode-coupling theory of the glass transition (MCT) for the tagged-particle density-correlation functions and the mean-squared displacement curves are compared quantitatively and in detail to results from Newtonian-…

统计力学 · 物理学 2009-11-10 Th. Voigtmann , A. M. Puertas , M. Fuchs

Effective interactions inherently encompass many-body effects that appear unified. Analyzing these in reverse, that is, separating them into contributions from pairs, triples, or larger groups, is typically intricate and seldom pursued.…

This paper organizes McMillan-Mayer theory, the potential distribution approach, and quasi-chemical theory to provide theory for the thermodynamic effects associated with longer spatial scales involving longer time scales, thus helping to…

化学物理 · 物理学 2013-10-16 W. Zhang , X. You , L. R. Pratt

Many-body interactions in water are known to be important but difficult to treat in atomistic models and often are included only as a correction. Polarizable models treat them explicitly, with long-range many-body potentials, within their…

化学物理 · 物理学 2023-02-21 David Abella , Giancarlo Franzese , Javier Hernández-Rojas

We study many-body correlation functions within various Fundamental Measure Theory (FMT) formulations and compare their predictions to Monte Carlo simulations of hard-sphere fluids. FMT accurately captures the qualitative behavior of three-…

化学物理 · 物理学 2025-10-30 Ilian Pihlajamaa , Teunike A. van de Pol , Liesbeth M. C. Janssen

We show that classical molecular density functional theory (MDFT), here in the homogeneous reference fluid approximation in which the functional is inferred from the properties of the bulk solvent, is a powerful new tool to study, at a…

We develop a variational approach at finite temperature that incorporates many-body correlation self-consistently. The grand potential is constructed in terms of Green's function expressed by the variational parameters. We apply this…

量子气体 · 物理学 2019-05-30 Akimitsu Kirikoshi , Wataru Kohno , Takafumi Kita

The density functional theory of nuclear structure provides a many-particle wave function that is useful for static properties, but an extension of the theory is necessary to describe correlation effects or other dynamic properties. Here we…

核理论 · 物理学 2009-11-11 Y. Alhassid , G. F. Bertsch , L. Fang , B. Sabbey

Knowledge of all correlation functions of a system is equivalent to solving the corresponding many-body problem. Already a finite set of correlation functions can be sufficient to describe a quantum many-body system if correlations…

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…

化学物理 · 物理学 2007-05-23 Lawrence R. Pratt , Randall A. LaViolette , Maria A. Gomez , Mary E. Gentile

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,…

化学物理 · 物理学 2022-06-27 Diego T. Gomez , Lawrence R. Pratt , Dilipkumar N. Asthagiri , Susan B. Rempe

We study the melting behavior of charged colloidal crystals, using a simulation technique that combines a continuous mean-field Poisson-Boltzmann description for the microscopic electrolyte ions with a Brownian-dynamics simulation for the…

软凝聚态物质 · 物理学 2009-11-13 J. Dobnikar , Y. Chen , R. Rzehak , H. H. von Grünberg

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…

化学物理 · 物理学 2021-05-14 Dilipkumar N. Asthagiri , Michael E. Paulaitis , Lawrence R. Pratt
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