Cooperation of N‐Heterocyclic Carbenes on a Gold Surface

Atomically precise tailoring of interface structures is crucial for developing functional materials. We demonstrate an N‐heterocyclic carbene (NHC) based molecular tool, which modifies the structure of a gold surface with atomic accuracy by the formation of gold nanorods. After adsorption on the gold surface, individual surface atoms are pulled out by the NHCs, generating single‐atom surface defects and mobile NHC‐Au species. Atomistic calculations reveal that these molecular “ballbots” can act as assembling tools to dislocate individual surface atoms. The predicted functionality of these carbene‐based complexes is confirmed by scanning tunneling microscopy measurements. Cooperative operation of these NHC‐Au species induces a step‐wise formation of gold nanorods. Consequently, the surface is re‐structured by a zipper‐type mechanism. Our work presents a foundation to utilize molecular‐based nanotools to design surface structures.