Journal of Chemical Physics, Vol.119, No.14, 7579-7590, 2003
Dynamics of dendrimer-based polymer networks
We present a theoretical study of polymer networks, formed by connecting dendritic building blocks (DBB's). We concentrate on the Rouse dynamics of such networks and perform our study in two steps, considering first single generalized dendrimers (GD's) and then networks formed by such DBB's. In GD's the functionality f of the inner branching points may differ from the functionality f(c) of the core. The GD's cover wide classes of macromolecules, such as the "classical" dendrimers (f(c)=f ), the dendritic wedges (f(c)=f-1), and the macromolecular stars (f(c)>2, f=2). Here we present a systematic, analytic way which allows us to treat the dynamics of individual GD's. Then, using a general approach based on regular lattices formed by identical cells (meshes) we study the dynamics of GD-based polymer networks. Using analytical and numerical methods we determine the storage and loss moduli, G(')(omega) and G(')(omega). In this way we find that the intradendrimer relaxation domain of G(')(omega) becomes narrower when M-cr, the number of connections between the neighboring DBB's, increases. This effect may be understood due to the exclusion of the longest DBB relaxation times from the spectrum of the network, given that the additional connections hinder the mobility of the peripheral DBB branches. We expect that such effects may be readily observed through appropriate mechanical experiments. (C) 2003 American Institute of Physics.