Self-Assembly Behavior of Amphiphilic Janus Dendrimers in Water: A Combined Experimental and Coarse-Grained Molecular Dynamics Simulation Approach

Abstract

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, the aggregation behavior in water of a second-generation bis-MPA JD was evaluated using experimental and computational methods. Dispersions of JDs in water were carried out using the thin-film hydration and ethanol injection methods. Resulting assemblies were characterized by dynamic light scattering, confocal microscopy, and atomic force microscopy. Furthermore, a coarse-grained molecular dynamics (CG-MD) simulation was performed to study the mechanism of JDs aggregation. The obtaining of assemblies in water with no interdigitated bilayers was confirmed by the experimental characterization and CG-MD simulation. Assemblies with dendrimersome characteristics were obtained using the ethanol injection method. The results of this study establish a relationship between the molecular structure of the JD and the properties of its aggregates in water. Thus, our findings could be relevant for the design of novel JDs with tailored assemblies suitable for drug delivery systems.

Screening Libraries of Amphiphilic Janus Dendrimers Based on Natural Phenolic Acids to Discover Monodisperse Unilamellar Dendrimersomes

“…With this new library of JDs and their self-assembled stable DSs, encapsulation, delivery, and change in structure during encapsulation and release are currently under investigation and will be reported in a different publication. Therefore, these JDs are expected to be utilized as important tools for nanomedicine − and synthetic cell biology.…”

The Martini Model in Materials Science

“…A large body of work has investigated the self‐assembly of different block copolymers in water or other solvents [ 123–136 ] Among these systems, the most studied with Martini are poloxamers [ 32,56,137–144 ] also known as pluronics, which are PEO–PPO–PEO amphiphilic triblock copolymers. Such polymers can form a wide range of aggregates ranging from bilayers, over micelles, to polymersomes, that is, synthetic vesicles, the latter ones being particularly studied for applications as nanocarrier devices for drug delivery.…”

The Martini Model in Materials Science

“…A large body of work has has investigated the selfassembly of different block copolymers in water or other solvents. [103][104][105][106][107][108][109][110][111][112][113] Among these systems, the most studied with Martini are poloxamers [114][115][116][117][118][119][120][121] also known as pluronics, which are PEO-PPO-PEO amphiphilic tri block copolymers. Such polymers can form a wide range of aggregates ranging from bilayers, over micelles, to polymersomes, that is, synthetic vesicles, the latter ones being particularly studied for applications as nanocarrier devices for drug delivery.…”