Multiscale modeling and simulation methods with applications to dendritic polymers

摘要

Dendrimers and hyperbranched polymers represent a novel class of structurally controlled macromolecules derived from a branches-upon-branches structural motif. The synthetic procedures developed for dendrimer preparation permit nearly complete control over the critical molecular design parameters, such as size, shape, surface/interior chemistry, flexibility, and topology. Dendrimers are well defined, highly branched macromolecules that radiate from a central core and are synthesized through a stepwise, repetitive reaction sequence that guarantees complete shells for each generation, leading to polymers that are mono-disperse. This property of dendrimers makes it particularly natural to coarsen interactions in order to simulate dynamic processes occurring at larger length and longer time scales. In this paper, we describe methods to construct 3-dimensional molecular structures of dendrimers (Continuous Configuration Boltzmann Biased direct Monte Carlo, CCBB MC) and methods towards coarse graining dendrimer interactions (NEIMO and hierarchical NEIMO methods) and representation of solvent dendrimer interactions through continuum solvation theories. Poisson-Boltzmann (PB) and Surface Generalized Born (SGB) methods. We will describe applications to PAMAM, stimuli response hybrid star-dendrimer polymers, and supra molecular assemblies crystallizing to A15 colloidal structure or Pm6m liquid crystals.