Particle self-assembly at liquid/liquid and liquid/air interfaces driven by capillary forces has gained a great deal of attention in chemistry, physics and biology for more than two decades. In this work, systematical investigation of cube orientation and capillary interactions for surface functionalized polystyrene (PS) microcubes that were fabricated via nanoimprint lithography (NIL) technique followed by self-assembled monolayer-based surface modification to control the wettability of five sides of the cubes are reported. With increasing the hydrophobicity of cube face, the orientation of the cubes at the water-air interface was found to be preferentially face up, edge up or vertex up, which resulted in the assembly of ‘flat plate’, ‘tilted linear’ and ‘close-packed hexagonal’ aggregates, driven by capillary force, respectively. In additional, based on ‘close-packed hexagonal’ aggregates, the asymmetric multifunctional 3D cell microenvironments were fabricated by introducing nanostructure and polymer brushes to the cube surfaces. The random assembly of different cubes from a library comprising microcubes that are pre-functionalized or surface-structured exclusively on their top surface opens a pathway to generate a multitude of different microenvironments in a massively parallel combinatorial manner, enabling future systematic structure-property relationship studies with cells.

In dynamic supramolecular chemistry, molecular cybernetics is fundamentally an emerging arena. Smart interactions and communicating molecular networks achieve to progress the responsive establishment of interdependent functions and cognitive autonomous control of off-equilibrium. This talk will review the progress of interconnected molecular machinery into functions such as control of luminescence1, catalysis2 and mechanically interlocked molecule having different mode of shuttling motion with impeccable reversibility. Some recent results from our lab on chemical fuel trigged autonomous multicomponent nanoswitch toggling will be presented.