Modulation doping and charge density wave transition in layered PbSe-VSe₂ ferecrystal heterostructures

Controlling charge carrier concentrations remains a major challenge in the application of quasi-two-dimensional materials. A promising approach is the modulation doping of transport channels via charge transfer from neighboring layers in stacked heterostructures. Ferecrystals, which are metastable layered structures created from artificial elemental precursors, are a perfect model system to investigate modulation doping, as they offer unparalleled freedom in the combination of different constituents and variable layering sequences. In this work, differently stacked combinations of rock-salt structured PbSe and VSe₂ were investigated using X-ray photoelectron spectroscopy. The PbSe layers act as electron donors in all heterostructures, with about 0.1 to 0.3 donated electrons per VSe₂ unit cell. While they initially retain their inherent semiconducting behavior, they themselves become metallic when combined with a larger number of VSe₂ layers, as evidenced by a change of the XPS core level lineshape. Additional analysis of the valence band structure was performed for selected stacking orders at different sample temperatures to investigate a predicted charge density wave (CDW) transition. While there appear to be hints of a gap opening, the data so far is inconclusive and the application of spatially resolved techniques such as scanning tunneling microscopy is encouraged for further studies.