Crystalline and electronic structure of single-layer TaS2_2

Single-layer TaS$_2$ is epitaxially grown on Au(111) substrates. The resulting two-dimensional crystals adopt the 1H polymorph. The electronic structure is determined by angle-resolved photoemission spectroscopy and found to be in excellent agreement with density functional theory calculations. The single layer TaS$_2$ is found to be strongly n-doped, with a carrier concentration of 0.3(1) extra electrons per unit cell. No superconducting or charge density wave state is observed by scanning tunneling microscopy at temperatures down to 4.7 K.Comment: 6 pages, 4 figure

Quasi-free-standing single-layer WS2 achieved by intercalation

Large-area and high-quality single-layer transition metal dichalcogenides can be synthesized by epitaxial growth on single-crystal substrates. An important advantage of this approach is that the interaction between the single-layer and the substrate can be strong enough to enforce a single crystalline orientation of the layer. On the other hand, the same interaction can lead to hybridization effects, resulting in the deterioration of the single-layer's native properties. This dilemma can potentially be solved by decoupling the single-layer from the substrate surface after the growth via intercalation of atoms or molecules. Here we show that such a decoupling can indeed be achieved for single-layer WS2 epitaxially grown on Ag(111) by intercalation of Bi atoms. This process leads to a suppression of the single-layer WS2-Ag substrate interaction, yielding an electronic band structure reminiscent of free-standing single-layer WS2

Pnictogens Allotropy and Phase Transformation during van der Waals Growth

Pnictogens have multiple allotropic forms resulting from their ns2 np3 valence electronic configuration, making them the only elemental materials to crystallize in layered van der Waals (vdW) and quasi-vdW structures throughout the group. Light group VA elements are found in the layered orthorhombic A17 phase such as black phosphorus, and can transition to the layered rhombohedral A7 phase at high pressure. On the other hand, bulk heavier elements are only stable in the A7 phase. Herein, we demonstrate that these two phases not only co-exist during the vdW growth of antimony on weakly interacting surfaces, but also undertake a spontaneous transformation from the A17 phase to the thermodynamically stable A7 phase. This metastability of the A17 phase is revealed by real-time studies unraveling its thickness-driven transition to the A7 phase and the concomitant evolution of its electronic properties. At a critical thickness of ~4 nm, A17 antimony undergoes a diffusionless shuffle transition from AB to AA stacked alpha-antimonene followed by a gradual relaxation to the A7 bulk-like phase. Furthermore, the electronic structure of this intermediate phase is found to be determined by surface self-passivation and the associated competition between A7- and A17-like bonding in the bulk. These results highlight the critical role of the atomic structure and interfacial interactions in shaping the stability and electronic characteristics of vdW layered materials, thus enabling a new degree of freedom to engineer their properties using scalable processes