How magnetism emerges in low-dimensional materials such as transition metal dichalcogenides at the monolayer limit is still an open question. Herein, we present a comprehensive study of the magnetic properties of single crystal and monolayer VSe2.0, both experimentally and ab initio. Magnetometry, X-ray magnetic circular dichrosim (XMCD) and ab initio calculations demonstrate that the charge density wave in bulk stoichiometric VSe2.0 causes a structural distortion with a strong reduction in the density of sates at the Fermi level, prompting the system towards a nonmagnetic state but on the verge of a ferromagnetic instability. In the monolayer limit, the structural rearrangement induces a Peierls distortion with the opening of an energy gap at the Fermi level and the absence of magnetic order. Control experiments on defect-induced VSe 2−δ single crystals show a breakdown of magnetism, discarding vacancies as a possible origin of magnetic order in VSe2.0. arXiv:1907.02034v1 [cond-mat.mes-hall]
Collective electronic states such as the charge density wave (CDW) order and superconductivity (SC) respond sensitively to external perturbations. Such sensitivity is dramatically enhanced in two dimensions (2D), where 2D materials hosting such electronic states are largely exposed to the environment. In this regard, the ineludible presence of supporting substrates triggers various proximity effects on 2D materials that may ultimately compromise the stability and properties of the electronic ground state. In this work, we investigate the impact of proximity effects on the CDW and superconducting states in single-layer (SL) NbSe 2 on four substrates of diverse nature, namely, bilayer graphene (BLG), SL-boron nitride (h-BN), Au(111), and bulk WSe 2 . By combining low-temperature (340 mK) scanning tunneling microscopy/spectroscopy and angle-resolved photoemission spectroscopy, we compare the electronic structure of this prototypical 2D superconductor on each substrate. We find that, even when the electronic band structure of SL-NbSe 2 remains largely unaffected by the substrate except when placed on Au(111), where a charge transfer occurs, both the CDW and SC show disparate behaviors. On the insulating h-BN/Ir(111) substrate and the metallic BLG/SiC(0001) substrate, both the 3 × 3 CDW and superconducting phases persist in SL-NbSe 2 with very similar properties, which reveals the negligible impact of graphene on these electronic phases. In contrast, these collective electronic phases are severely weakened and even absent on the bulk insulating WSe 2 substrate and the metallic single-crystal Au(111) substrate. Our results provide valuable insights into the fragile stability of such electronic ground states in 2D materials.
Bulk and single-layer 2H-NbSe 2 exhibit identical charge density wave order (CDW) with a quasi-commensurate 3×3 superlattice periodicity. Here we combine scanning tunnelling microscopy (STM) imaging at T = 1 K of 2H-NbSe 2 with firstprinciples density functional theory (DFT) calculations to investigate the structural atomic rearrangement of this CDW phase. Our calculations for single-layers reveal that six different atomic structures are compatible with the 3×3 CDW distortion, although all of them lie on a very narrow energy range of at most 3 meV per formula unit, suggesting the coexistence of such structures. Our atomically resolved STM images of bulk 2H-NbSe 2 unambiguously confirm this by identifying two of these structures. Remarkably, these structures differ from the X-ray crystal structure reported for the bulk 3×3 CDW which, in fact, is also one of the six DFT structures located for the single-layer. Our calculations also show that due to the minute energy difference between the different phases, the ground state of the 3×3 CDW could be extremely sensitive to doping, external strain or internal pressure within the crystal. The presence of multi-phase CDW order in 2H-NbSe 2 may provide further understanding of its low temperature state and the competition between different instabilities.
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