相关论文: Accurate Evaluation of Charge Asymmetry in Aqueous…

We study the chemical potential of water as a function of charge based on perturbation theory. By calculating the electrostatic-energy fluctuations of two states (fully charged and uncharged) we are able to determine accurate values for the…

Controlling electrochemical reactivity requires a detailed understanding of the charging behavior and thermodynamics of the electrochemical interface. Experiments can independently probe the overall charge response of the electrochemical…

Determining the solvation free energies of single ions in water is one of the most fundamental problems in physical chemistry and yet many unresolved questions remain. In particular, the ability to decompose the solvation free energy into…

Simplified, classical models of water are an integral part of atomistic molecular simulations, especially in biology and chemistry where hydration effects are critical. Yet, despite several decades of effort, these models are still far from…

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…

The effects of size and charge asymmetry on the gas-liquid critical parameters of a primitive model (PM) of ionic fluids are studied within the framework of the statistical field theory based on the collective variables method. Recently,…

Anions generally associate more favorably with the air-water interface than cations. In addition to solute size and polarizability, the intrinsic structure of the unperturbed interface has been discussed as an important contributor to this…

Interpretation of the X-ray spectra of water as evidence for its asymmetric structure has challenged the conventional symmetric nearly-tetrahedral model and initiated an intense debate about the order and symmetry of the hydrogen bond…

Why kinetically stable oil droplets in water spontaneously acquire a negative charge remains one of the most vigorously debated questions in interfacial science. Here, we combine neural-network based deep potential molecular dynamics with a…

The hydration structure of Ba^{2+} ion is important for understanding blocking mechanisms in potassium ion channels. Here, we combine statistical mechanical theory, ab initio molecular dynamics simulations, and electronic structure methods…

Liquid-liquid phase separation has emerged as one of the important paradigms in the chemical physics as well as biophysics of charged macromolecular systems. We elucidate an equilibrium phase separation mechanism based on charge regulation,…

The structure of polar liquids and electrolytic solutions, such as water and aqueous electrolytes, at interfaces underlies numerous phenomena in physics, chemistry, biology, and engineering. In this work, we develop a continuum theory that…

Second-Harmonic Scatteringh (SHS) experiments provide a unique approach to probe non-centrosymmetric environments in aqueous media, from bulk solutions to interfaces, living cells and tissue. A central assumption made in analyzing SHS…

Dynamic structuring of water is a key player in a large class of processes underlying biochemical and technological developments today, the latter often involving electric fields. However, the anisotropic coupling between the water…

Chemical thermodynamic models of solvent and solute activities predict the equilibrium behaviour of aqueous solutions. How-ever, these models are semi-empirical. They represent micro-scale ion and solvent behaviours that control the…

We generalize the predictions for attractions between over-all neutral surfaces induced by charge fluctuations/correlations to non-uniform systems that include dielectric discontinuities, as is the case for mixed charged lipid membranes in…

Within the framework of a functional integral formalism incorporating ionic charge and hard-core (HC) interactions on an equal footing, we formulate a unified theory of equilibrium thermodynamics and ion association in charged solutions.…

By combining accurate liquid-vapor coexistence and heat-capacity data, we have unambiguously separated two non-analytical contributions of liquid-gas asymmetry in fluid criticality and proved the validity of "complete scaling" [Fisher et…

Neutron scattering and molecular dynamics studies were performed on a concentrated aqueous tetramethylammonium (TMA) chloride solution to gain insight into the hydration shell structure of TMA, which is relevant for understanding its…

The organization of water molecules and ions between charged mineral surfaces determines the stability of colloidal suspensions and the strength of phase-separated particulate gels. In this article we assemble a density functional that…