Dynamics theory for molecular liquids based on an interaction site model

Abstract

Dynamics theories for molecular liquids based on an interaction site model have been developed over the past few decades and proved to be powerful tools to investigate various dynamical phenomena. In many of these theories, equations of time correlation functions are formulated by using the Zwanzig-Mori projection operator. Since algebriac equations are directly treated in these statistical mechanical approaches, the obtained dynamical properties are essentially free from statistical error. This perspective presents the theoretical framework of such theories and their applications, including visualization of diffusion processes, collective excitations, solvation dynamics, transport properties, and diffusion controlled reactions.

Solvent Distribution Effects on Quantum Chemical Calculations with Quantum Computers

“…To determine the solvation structure intuitively, we first visualized its 3D distribution functions g v ( r ) in Figure , resulting from the 3D-RISM-VQE­(8e, 6o) calculation with the 6-31G* basis set. The shape of the distribution functions g v ( r ) is similar to the previous studies. ,− The arched bilayered solvent shell near the solute oxygen and on the opposite side of the two hydrogens of the solute can be identified; the inside layer is g H ( r ) and the outside is g O ( r ). Two other distributions of g O ( r ) and g H ( r ) are situated around the two hydrogen atoms and on the opposite side of the solute oxygen.…”

Structural Origin of Shear Viscosity of Liquid Water

“…To examine the coupling between the dynamics of the stress tensor and the liquid structure, the cross-correlation function between the shear stress and the two-body density at different times is defined as Here, the two-body density is defined as where ρ̃ α ( q ) denotes the density field of the site α at the wavevector q in the reciprocal space. The interaction-site description of the dynamics of molecular liquids is employed here, where the reorientational motion is described as the coupled diffusion of different sites . The interaction site refers to a real or united atom, and a water molecule is composed of one oxygen and two hydrogen sites, namely, O, H, and H′.…”

“…The interaction-site description of the dynamics of molecular liquids is employed here, where the reorientational motion is described as the coupled diffusion of different sites. 10 The interaction site refers to a real or united atom, and a water molecule is composed of one oxygen and two hydrogen sites, namely, O, H, and H′. The trivial orientational dependence is factored out in the definition of eq 2 to define ρ (2) η,αγ (q, t) as a scalar function.…”

Solvation dynamics on the diffusion timescale elucidated using energy-represented dynamics theory

“…The dynamics theories based on the integral equation theory of molecular liquids with the interaction-site representation [27][28][29] have been also widely used to investigate the solvation dynamics of the various solutes in molecular liquids. [30][31][32][33][34][35][36][37][38][39][40] The governing equations have a mathematically closed form for both the static and dynamic properties of solutions, and hence information on the dynamics can be obtained by solving the equations in an algebraic manner, meaning that the obtained results are free from the sampling problem. [41][42][43][44][45] The application of these theories to the solvation dynamics is possible with the aid of a modified linear response theory 32,34 or time-dependent density functional theory (TD-DFT) of liquids.…”