Computer simulation studies of self-assembling macromolecules

Coarse-grained (CG) molecular models are now widely used to understand the structure and functionality of macromolecular self-assembling systems. In the last few years, significant efforts have been devoted to construct quantitative CG models based on data from molecular dynamics (MD) simulations with more detailed all-atom (AA) intermolecular force fields as well as experimental thermodynamic data. We review some of the recent progress pertaining to the MD simulation of self-assembling macromolecular systems, using as illustrations the application of CG models to probe surfactant and lipid self-assembly including liposome and dendrimersome formation as well as the interaction of biomembranes with nanoparticles.

► Chemically accurate coarse-grained molecular models allow quantitative simulation of macromolecular self-assembly. ► Novel free energy methods are key in characterizing the stability of self-assembled structures. ► Predictive simulation is illustrated with liposomes, polymersomes, and dendrimersomes. ► Nanoparticle assembly in liposomes is complex, depending on the thickness and curvature of the membrane. ► Membrane fusion is one of the frontiers of coarse-grained molecular simulation.