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Abstract Nature provides many examples of the benefits of nanoscopic surface structures in areas of adhesion and antifouling. Herein, the design, fabrication, and characterization of liquid crystal elastomer (LCE) films are presented with nanowire surface structures that exhibit tunable stimuli‐responsive deformations and enhanced adhesion properties. The LCE films are shown to curl toward the side with the nanowires when stimulated by heat or organic solvent vapors. In contrast, when a droplet of the same solvent is placed on the film, it curls away from the nanowire side due to nanowire‐induced capillary forces that cause unequal swelling. This characteristic curling deformation is shown to be reversible and can be optimized to match curved substrates, maximizing adhesive shear forces. By using chemical modification, the LCE nanowire films can be given underwater superoleophobicity, enabling oil repellency under a range of harsh conditions. This is combined with the nanowire‐induced frictional asymmetry and the reversible shape deformation to create an underwater droplet mixing robot, capable of performing chemical reactions in aqueous environments. These findings demonstrate the potential of nanowire‐augmented LCE films for advanced applications in soft robotics, adaptive adhesion, and easy chemical modification, with implications for designing responsive materials that integrate mechanical flexibility with surface functionality. 

Abstract Two-dimensional (2D) superlattices, formed by stacking sublattices of 2D materials, have emerged as a powerful platform for tailoring and enhancing material properties beyond their intrinsic characteristics. However, conventional synthesis methods are limited to pristine 2D material sublattices, posing a significant practical challenge when it comes to stacking chemically modified sublattices. Here we report a chemical synthesis method that overcomes this challenge by creating a unique 2D graphene superlattice, stacking graphene sublattices with monodisperse, nanometer-sized, square-shaped pores and strategically doped elements at the pore edges. The resulting graphene superlattice exhibits remarkable correlations between quantum phases at both the electron and phonon levels, leading to diverse functionalities, such as electromagnetic shielding, energy harvesting, optoelectronics, and thermoelectrics. Overall, our findings not only provide chemical design principles for synthesizing and understanding functional 2D superlattices but also expand their enhanced functionality and extensive application potential compared to their pristine counterparts.