Dual-Interface-Mediated Tunable Self-Assembly of 2D Periodic Nanostructures and DNA-Driven Reconstructions

To accurately regulate and dynamically reconstruct two-dimensional (2D) periodic nanostructures is a great challenge but is of significance for the development of functional integrated devices. Here, through both chemical and physical modifications of the lithographical template surface, a patterned dual interface of active molecular binding sites was created, enabling flexible regulation of self-assembly of DNA-decorated Au nanoparticles to generate 2D periodic nanostructures that feature distinct patterns. As a proof of concept, we realized three types of periodic structures of Au nanoparticles, including inverse structures, ring arrays, and island arrays, through template-confined and regioselective self-assembly processes. Besides, controllable reconstruction of the periodic nanostructures was demonstrated through DNA-dictated assembly of Au nanoparticles on the surface, offering a pathway to actively manipulate their light-matter interactions. These findings highlight the potential of heterogeneous molecular patterning of the template surface in achieving more intricate periodic nanostructures via surface-mediated assembly of nanoparticles over large areas.