Nontrivial Doping Evolution of Electronic Properties in Ising‐Superconducting Alloys

Transition metal dichalcogenides offer unprecedented versatility to engineer 2D materials with tailored properties to explore novel structural and electronic phase transitions. In this work, the atomic‐scale evolution of the electronic ground state of a monolayer of Nb1−δMoδSe2 across the entire alloy composition range (0 < δ < 1) is investigated using low‐temperature (300 mK) scanning tunneling microscopy and spectroscopy (STM/STS). In particular, the atomic and electronic structure of this 2D alloy throughout the metal to semiconductor transition (monolayer NbSe2 to MoSe2) is studied. The measurements enable extraction of the effective doping of Mo atoms, the bandgap evolution and the band shifts, which are monotonic with δ. Furthermore, it is demonstrated that collective electronic phases (charge density wave and superconductivity) are remarkably robust against disorder and further shown that the superconducting TC changes non‐monotonically with doping. This contrasting behavior in the normal and superconducting state is explained using first‐principles calculations. Mo doping is shown to decrease the density of states at the Fermi level and the magnitude of pair‐breaking spin fluctuations as a function of Mo content. These results paint a detailed picture of the electronic structure evolution in 2D TMD alloys, which is of utmost relevance for future 2D materials design.