Definitions of local density in density-dependent potentials for mixtures.

Density-dependent potentials are frequently used in materials simulations because of their approximate description of many-body effects at minimal computational cost. However, in order to apply such models to multicomponent systems, an appropriate definition of total local particle density is required. Here, we discuss two definitions of local density in the context of many-body dissipative particle dynamics. We show that only a potential which combines local densities from all particle types in its argument gives physically meaningful results for all composition ratios. Drawing on the ideas from metal potentials, we redefine local density such that it can accommodate different intertype interactions despite the constraint to keep the main interaction parameter constant, known as Warren's no-go theorem, and generalize the many-body potential to heterogeneous systems. We then show via simulation how liquid-liquid and liquid-solid coexistence can arise just by tuning the interaction parameters.

Invariance of experimental observables with respect to coarse-graining in standard and many-body dissipative particle dynamics.

Dissipative particle dynamics (DPD) is a well-established mesoscale simulation method. However, there have been long-standing ambiguities regarding the dependence of its (purely repulsive) force field parameter on temperature as well as the variation of the resulting experimental observables, such as diffusivity or surface tension, with coarse-graining (CG) degree. Here, we rederive the temperature dependence of DPD interaction parameter and revisit the role of the CG degree in standard DPD simulations. Consequently, we derive a scaling of the input variables that renders the system properties invariant with respect to CG degree and illustrate the versatility of the method by computing the surface tensions of binary solvent mixtures. We then extend this procedure to many-body dissipative particle dynamics and, by computing surface tensions of the same mixtures at a range of CG degrees, demonstrate that this newer method, which has not been widely applied so far, is also capable of simulating complex fluids of practical interest.