Robust Behavior of Charge Density Wave Quantum Motif Star‐of‐David in 2D NbSe₂ Nanocrystals

Abstract Charge density wave (CDW) is a typical collective phenomenon, and the phase change is generally accompanied by electronic transition with potential device applications. For the continuous miniaturization of devices, it is important to investigate the size effect down to the nanoscale. In this work, single‐layer (SL) 1T‐NbSe₂ islands provide an ideal research platform to investigate the size effect on CDW arrangement and electronic states. The CDW motifs (Star‐of‐David [SOD]) at the island border are along the edge, and those at the interior tend to arrange in a triangular lattice for islands as small as 5 nm. Interestingly, in some small islands, the SOD clusters rearrange into a square‐like lattice, and each SOD cluster remains robust as a quantum motif, both in the sense of geometry and electronic structures. Moreover, the electronic structure at the center of the small islands is downwards shifted compared to the big islands, explained by the spatial extension of the band bending originating from the edge of the islands. These findings reveal the robust behavior of CDW motifs down to the nanoscale and provide new insights into the size‐limiting effect on 2D2D CDW ordering and electronic states down to a few nanometer extremes.