Osmolyte Effects: Impact on the Aqueous Solution around Charged and Neutral Spheres

We have performed atomistic molecular dynamics simulations to study the solvation characteristics of model spheres for low concentrations of urea and hydroxyectoine in aqueous solution. The spheres are either positively or negatively charged with a valency of one or charge neutral. Our results illustrate that the presence of osmolytes influences the solvation properties of the spheres significantly. We have conducted a detailed investigation of water properties like the mean dipolar relaxation times, water orientation parameters around the spheres, dielectric constants, preferential binding behavior, water self-diffusion coefficients, and free energies of solvation by thermodynamic integration to study the influence of osmolytes in detail. Our findings indicate that several factors like the charge of the spheres as well as the characteristics of the osmolytes significantly influence the thermodynamic and dynamic properties of the local water shell and the solvation process with regard to varying enthalpic and entropic contributions.