相关论文: The hydration free energy of water
A new molecular dynamics model in which the point charges on atomic sites are allowed to fluctuate in response to the environment is developed and applied to water. The idea for treating charges as variables is based on the concept of…
Recent experimental results suggest that a particular hydrodynamic theory describes charge fluctuations at long wavelengths in the square-lattice Hubbard model. Due to the continuity equation, the correlation functions for the charge and…
We present a new interatomic potential for water captured in a charge-transfer embedded atom method (EAM) framework. The potential accounts for explicit, dynamical charge transfer in atoms as a function of the local chemical environment. As…
The frequency-dependent impedance is a fundamental property of electrical components. We show that it can be determined from the equilibrium dynamical fluctuations of the electrode charge in constant-potential molecular simulations,…
The fluctuations of the charge on an electrode contain information on the microscopic correlations within the adjacent fluid and their effect on the electronic properties of the interface. We investigate these fluctuations using molecular…
The hydration free energies of ions exhibit an approximately quadratic dependence on the ionic charge, as predicted by the Born model. We analyze this behavior using second-order perturbation theory. This provides effective methods to…
The microscopic description of the local structure of water remains an open challenge. Here, we adopt an agnostic approach to understanding water's hydrogen bond network using data harvested from molecular dynamics simulations of an…
Charge hydration asymmetry (CHA)--a characteristic dependence of hydration free energy on the sign of the solute charge--quantifies the asymmetric response of water to electric field at microscopic level. Accurate estimates of CHA are…
The open water surface is known to be charged. Yet, the magnitude of the charge and the physical mechanism of the charging remain unclear, causing heated debates across the scientific community. Here we directly measure the charge Q of…
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…
A new classical interaction potential for water simulations is presented. Water is modeled as a fully dissociable set of atoms with a point dipole, determined self-consistently, on every oxygen atom. The oxygen polarizability is not fixed…
We present an accurate equation of state for water based on a simple microscopic Hamiltonian, with only four parameters that are well-constrained by bulk experimental data. With one additional parameter for the range of interaction, this…
The results of molecular dynamics simulations of the properties of water in an aqueous ionic solution close to an interface with a model metallic electrode are described. In the simulations the electrode behaves as an ideally polarizable…
Accurate calculation of free energies and their derivatives is central to assessing the thermodynamic stability of molecular and particulate systems across length scales. Yet such quantities can be difficult to compute reliably in strongly…
In this work we develop a new classical perturbation theory for water which incorporates the transition to tetrahedral symmetry in both the dispersion and hydrogen bonding contributions to the free energy. This transition is calculated…
The surface or contact potential at the water liquid-vapor interface is discussed in relation to determinations of absolute ion hydration free energies and distributions of ions near the interface. It is shown that, rather than the surface…
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…
Can we avoid molecular dynamics simulations to estimate the electrostatic interaction between charged objects separated by a nanometric distance in water? To answer this question, we develop a continuous model for the dielectric properties…
Nuclear quantum effects, such as zero-point energy and tunneling, cause significant changes to the structure and dynamics of hydrogen bonded systems such as liquid water. However, due to the current inability to simulate liquid water using…
Different schemes for the treatment of long-ranged electrostatic interactions will be examined for water simulations using the polarizable fluctuating charge potential. Several different methods are compared, including Ewald sums, potential…