Self-Assembly behavior of amphiphilic janus dendrimers in water: a combined experimental and coarse-grained molecular dynamics simulation approach
Elizondo García, Mariana Estefanía
MetadataShow full item record
Amphiphilic Janus dendrimers (JDs) are repetitively branched molecules with hydrophilic and hydrophobic components that self-assemble in water to form a variety of morphologies, including vesicles analogous to liposomes with potential pharmaceutical and medical application. To date, the self-assembly of JDs has not been fully investigated thus it is important to gain insight into its mechanism and dependence on JDs’ molecular structure. In this study, a series of amphiphilic JDs with variations in their core and branching pattern was synthesized and its aggregation behavior in water was evaluated using experimental and computational methods. JDs were obtained from 2,2-bis(hydroxymethyl)propionic acid, myristic acid and different glycols. Dispersions of JDs in water were carried out using the thin-film hydration, solvent injection methods and by microfluidics, using double emulsion drops with ultrathin shells as templates. Furthermore, a coarse-grained molecular dynamics (CG-MD) simulation was performed to study the mechanism of JDs aggregation. The resulting assemblies were characterized by optical microscopy, dynamic light scattering, confocal microscopy, and atomic force microscopy. The obtaining of assemblies in water with no interdigitated bilayers was confirmed by the experimental characterization and CG-MD simulation for one of the dendrimers. Assemblies with dendrimersome characteristics were obtained using the solvent injection method. Also, monodisperse nanometric assemblies were obtained by this method. The use of microfluidics enables the production of giant dendrimersomes from highly hydrophobic JDs, even when the dendrimers did not form vesicles using the thin-film hydration method. The results of this study establish a relationship between the molecular structure of the JDs and the properties of its aggregates in water. These results could be relevant for the design of novel JDs with tailored assemblies suitable for drug delivery systems. In addition, this study offers an approach to produce dendrimersomes in a more controlled way.