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 Co_1/3NbS₂, 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 a_1g 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.