Tunable Single-Atomic Charges on a Cleaved Intercalated Transition Metal Dichalcogenide

Control of a single ionic charge state by altering the number of bound electrons has been considered as an ultimate testbed for atomic charge-induced interactions and manipulations, and such subject has been studied in artificially deposited objects on thin insulating layers. We demonstrate that an entire layer of controllable atomic charges on a periodic lattice can be obtained by cleaving metallic Co1/3NbS2, an intercalated transition metal dichalcogenide. We identified a metastable charge state of Co with a different valence and manipulated atomic charges to form a linear chain of the metastable charge state. Density functional theory investigation reveals that the charge state is stable due to a modified crystal field at the surface despite the coupling between NbS2 and Co via a1g orbitals. The idea can be generalized to other combinations of intercalants and base matrices, suggesting that they can be a new platform to explore single-atom-operational 2D electronics/spintronics.