Theoretical Method of Calculating Solvent Nonequilibrium Effect on Solute Movement

We formulate a theoretical method for studying the solvent particle dynamics around a moving solute, using time-dependent density functional theory. The theoretical method is applied to the insertion process of a large sphere into a cylindrical vessel immersed in solvent particles. For various velocities of the large sphere, we calculate the nonequilibrium spatial distribution of number density of solvent particles. We find a nonequilibrium effect on the distribution, which is characterized by the total number of solvent particles inside of the vessel. The number is 32.5% larger for a velocity of DS/2dS than for the equilibrium state, where, dS and DS are the diameter and diffusion coefficient of a solvent particle, respectively.