Domain-Dependent Surface Adhesion in Twisted Few-Layer Graphene

<br/>Twisted van der Waals heterostructures are a highly tunable platform due to the many degrees of freedom available for controlling their electronic and chemical properties. Here, we focus on the local stacking order of low-degree twisted graphene heterostructures as a platform for manipulating the surface chemistry of this class of materials. We report the emergence and engineering of stacking domain-dependent surface adhesion in twisted few-layer graphene. Minimally twisted double bi- and tri-layer graphene heterostructures were fabricated and imaged using mid-infrared near-field optical microscopy and atomic force microscopy to identify rhombohedral and Bernal stacking domains. We then observed that metallic nanoparticles and liquid water exhibit a domain-selective adhesion on these heterostructures, with preference for the rhombohedral stacking configurations. Finally, we used an atomic force microscope to manipulate nanoparticles located at certain stacking domains, resulting in a local reconfiguration of the moiré superlattice near the nanoparticles at the μm-scale. Our findings establish a new approach to controlling moiré chemistry and nanoengineering.