Ordered nanoparticle self-assembly driven by membrane curvature: computational insights

Owing to their tunable optical, electronic, magnetic, and mechanical properties, nanostructured materials assembled from nanoparticles (NPs) have attracted growing interest. Their collective behavior is governed by NP size, shape, surface chemistry, and spatial organization. Bottom-up self-assembly provides a versatile fabrication route, typically requiring a soft medium to mediate NP interactions. Lipid membranes are particularly attractive scaffolds for NP assembly due to their low dimensionality, fluidity, and elasticity. NP adhesion to lipid membranes induces curvature deformation extending beyond the particle size. Overlap of these deformations generates effective multibody, curvature-mediated interactions that can drive NP self-assembly. This review summarizes recent coarse-grained molecular dynamics studies of NP self-assembly on planar lipid membranes and vesicles. Uniform NPs adhering to the inner leaflet of vesicles form quasi-two-dimensional, star-like nanoclusters stabilized by repulsive curvature-mediated interactions, whereas NPs on planar membranes or outer leaflet of vesicles assemble into linear close-packed chains. Introducing surface anisotropy through Janus modification overcomes these limitations by suppressing close-packed aggregation and endocytosis. Janus NPs on lipid vesicles form deltahedral nanoclusters, including some Platonic solids. On planar membranes, they assemble into triangular superlattices. Geometric anisotropy expands the range of accessible membrane-mediated assemblies. These findings highlight lipid membranes as adaptive scaffolds for reconfigurable nanostructures without direct NP-NP binding.