2D Materials by Design: Intercalation of Cr or Mn between two VSe₂ van der Waals Layers

Insertion of metal layers between layered transition-metal dichalcogenides (TMDs) enables the design of new pseudo-2D nanomaterials. The general premise is that various metal atoms may adopt energetically favorable intercalation sites between two TMD sheets. These covalently bound metals arrange in metastable configurations and thus enable the controlled synthesis of nanomaterials in a bottom-up approach. Here, this method is demonstrated by the insertion of Cr or Mn between VSe₂ layers. Vacuum-deposited transition metals diffuse between VSe₂ layers with increasing concentration, arranging in ordered phases. The Cr³⁺ or Mn²⁺ ions are in octahedral coordination and thus in a high-spin state. Measured and computed magnetic moments are high for dilute Cr atoms, but with increasing Cr concentration the average magnetic moment decreases, suggesting antiferromagnetic ordering between Cr ions. The many possible combinations of transition metals with TMDs form a library for exploring quantum phenomena in these nanomaterials.