Regulation of Interfacial Anchoring Orientation of Anisotropic Nanodumbbells

[Image: see text] Nanoparticles exhibiting geometrical and chemical anisotropies hold promise for environmentally responsive materials with tunable mechanical properties. However, a comprehensive understanding of their interfacial behaviors remains elusive. In this paper, we control the interfacial anchoring orientation of polystyrene nanodumbbells by adjusting interparticle forces. The film nanostructure is characterized by the orientation angle analysis of individual dumbbells from cross-sectional EM data: dumbbells undergo orientation transitions from a distinctive horizontal bilayer to an isotropic anchoring when electrostatic repulsion is suppressed by either an ionic strength increase or surface amine-modification. This anchoring orientation influences the film’s mechanical properties and foam stability, as investigated by a 2D isotherm and dark/bright-field microscopy measurements. Our findings highlight the potential for precise control of supra-colloidal structures by modulating particle alignment, paving the way for smart delivery systems.