Vesicle Morphogenesis in Amphiphilic Triblock Copolymer Solutions

Coarse-grained molecular dynamics simulations are employed to investigate the spatiotemporal evolution of vesicles (polymersomes) through the self-assembly of randomly distributed amphiphilic BAB triblock copolymers with hydrophilic A and hydrophobic B blocks in an aqueous solution. The vesiculation...

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Bibliographic Details
Published in:Colloids and interfaces 2024-06, Vol.8 (3), p.29
Main Authors: Liu, Senyuan, Samie, Mohammad Sadegh, Sureshkumar, Radhakrishna
Format: Article
Language:English
Subjects:
Aqueous solutions
Block copolymers
Cages
Configurations
Copolymers
Distribution (Probability theory)
Equilibrium
Hydrophobicity
information entropy
micelle
Micelles
Molecular dynamics
Monte Carlo simulation
Morphology
NMR
Nuclear magnetic resonance
Polymers
polymersome
Self-assembly
Simulation methods
Solvents
triblock copolymer
vesicle
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Summary:Coarse-grained molecular dynamics simulations are employed to investigate the spatiotemporal evolution of vesicles (polymersomes) through the self-assembly of randomly distributed amphiphilic BAB triblock copolymers with hydrophilic A and hydrophobic B blocks in an aqueous solution. The vesiculation pathway consists of several intermediate structures, such as an interconnected network of copolymer aggregates, a cage of cylindrical micelles, and a lamellar cage. The cage-to-vesicle transition occurs at a constant aggregation number and practically eliminates the hydrophobic interfacial area between the B block and solvent. Molecular reorganization underlying the sequence of morphology transitions from a cage-like aggregate to a vesicle is nearly isentropic. The end-to-end distances of isolated copolymer chains in solution and those within a vesicular assembly follow lognormal probability distributions. This can be attributed to the preponderance of folded chain configurations in which the two hydrophobic end groups of a given chain stay close to each other. However, the probability distribution of end-to-end distances is broader for chains within the vesicle as compared with that of a single chain. This is due to the swelling of the folded configurations within the hydrophobic bilayer. Increasing the hydrophobicity of the B block reduces the vesiculation time without qualitatively altering the self-assembly pathway.
ISSN:2504-5377
2504-5377
DOI:10.3390/colloids8030029