Magnetic correlations in single-layer NbSe2.

By means of spin-resolved density functional theory calculations using both atomic orbitals and plane-wave basis codes, we study the electronic and magnetic ground state of single-layer NbSe2. We find that, for all the functionals considered, the most stable solution in this 2D superconductor is the ferrimagnetic ground state with a magnetic moment of 1.09 µB at the Nb atoms and of 0.05 µB at the Se atoms pointing in the opposite direction. Our calculations show that the ferrimagnetic state precludes the development of charge density wave (CDW) order and their coexistence in the single-layer limit, unless graphene is considered as a substrate. The spin-resolved calculated DOS, a key fingerprint of the electronic and magnetic structure of a material, unambiguously reproduces the experimental DOS measured by scanning tunneling spectroscopy (STS) in single-layer NbSe2. Our work sets magnetism into play in this prototypical correlated 2D material, which is crucial to understand the formation mechanisms of 2D superconductivity and charge density wave order.