Kondo lattices are ideal testbeds for the exploration of heavy-fermion quantum phases of matter. While our understanding of Kondo lattices has traditionally relied on complex bulk f-electron systems, transition metal dichalcogenide heterobilayers have recently emerged as simple, accessible and tunable 2D Kondo lattice platforms where, however, their ground state remains to be established. Here we present evidence of a coherent ground state in the 1T/1H-TaSe2 heterobilayer by means of scanning tunneling microscopy/spectroscopy at 340 mK. Our measurements reveal the existence of two symmetric electronic resonances around the Fermi energy, a hallmark of coherence in the spin lattice. Spectroscopic imaging locates both resonances at the central Ta atom of the charge density wave of the 1T phase, where the localized magnetic moment is held. Furthermore, the evolution of the electronic structure with the magnetic field reveals a non-linear increase of the energy separation between the electronic resonances. Aided by ab initio and auxiliary-fermion mean-field calculations, we demonstrate that this behavior is inconsistent with a fully screened Kondo lattice, and suggests a ground state with magnetic order mediated by conduction electrons. The manifestation of magnetic coherence in TMD-based 2D Kondo lattices enables the exploration of magnetic quantum criticality, Kondo breakdown transitions and unconventional superconductivity in the strict two-dimensional limit.
Chemical substitution is a promising route for the exploration of a rich variety of doping- and/or disorder-dependent collective phenomena in low-dimensional quantum materials. Here we show that transition metal dichalcogenide alloys are ideal platforms to this purpose. In particular, we demonstrate the emergence of superconductivity in the otherwise metallic single-layer TaSe2 by minute electron doping provided by substitutional W atoms. We investigate the temperature and magnetic field dependence of the superconducting state of Ta1-δWδSe2 with electron doping (δ) using variable temperature (0.34–4.2 K) scanning tunneling spectroscopy (STS). We unveil the emergence of a superconducting dome spanning 0.003 < δ < 0.03 with a maximized critical temperature of 0.9 K, a significant increase from that of bulk TaSe2 (TC = 0.14 K). Superconductivity emerges from an increase of the density of states (DOS) as the Fermi surface approaches a van Hove singularity due to doping. Once the singularity is reached, however, the DOS decreases with δ, which gradually weakens the superconducting state, thus shaping the superconducting dome. Lastly, our doping-dependent measurements suggest the development of a Coulomb glass phase triggered by disorder due to W dopants.
9 June 2021 in Journal of Physics: Condensed Matter
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 NbSe 2 . We find that, for all the functionals considered, the most stable solution in this two-dimensional (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 density of states (DOS), a key fingerprint of the electronic and magnetic structure of a material, unambiguously reproduces the experimental DOS measured by scanning tunneling spectroscopy in single-layer NbSe 2 . Our work sets magnetism into play in this prototypical correlated 2D material, which is crucial to understand the formation mechanisms of 2D superconductivity and CDW order.