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Register a new userVan der Waals heteroepitaxial growth of monolayer Sb in puckered honeycomb structure
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Atomically thin two-dimensional (2D) crystals have gained tremendous attentions owing to their potential impacts to the future electronics technologies, as well as the exotic phenomena emerging in these materials. Monolayer of {alpha} phase Sb ({alpha}-antimonene) that shares the same puckered structure as black phosphorous, has been predicted to be stable with precious properties. However, the experimental realization still remains challenging. Here, we successfully grow high-quality monolayer {alpha}-antimonene, with the thickness finely controlled. The {alpha}-antimonene exhibits great stability upon exposure to air. Combining scanning tunneling microscope, density functional theory calculations and transport measurement, it is found that the electron band crossing the Fermi level exhibits a linear dispersion with a fairly small effective mass, and thus a good electrical conductivity. All of these properties make the {alpha}-antimonene promising in the future electronic applications.
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Puckered honeycomb Sb monolayer, the structural analog of black phosphorene, has been recently successfully grown by means of molecular beam epitaxy. However, little is known to date about the growth mechanism for such puckered honeycomb monolayer. In this study, by using scanning tunneling microscopy in combination with first-principles density functional theory calculations, we unveil that the puckered honeycomb Sb monolayer takes a kinetics-limited two-step growth mode. As the coverage of Sb increases, the Sb atoms firstly form the distorted hexagonal lattice as the half layer, and then the distorted hexagonal half-layer transforms into the puckered honeycomb lattice as the full layer. These results provide the atomic-scale insight in understanding the growth mechanism of puckered honeycomb monolayer, and can be instructive to the direct growth of other monolayers with the same structure.
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.
Research on two-dimensional materials has expanded over the past two decades to become a central theme in condensed matter research today. Significant advances have been made in the synthesis and subsequent reassembly of these materials using mechanical methods into a vast array of hybrid structures with novel properties and ever-increasing potential applications. The key hurdles in realizing this potential are the challenges in controlling the atomic structure of these layered hybrid materials and the difficulties in harnessing their unique functionality with existing semiconductor nanofabrication techniques. Here we report on high-quality van der Waals epitaxial growth and characterization of a layered topological insulator on freestanding monolayer graphene transferred to different mechanical supports. This templated synthesis approach enables direct interrogation of interfacial atomic structure of these as-grown hybrid structures and opens a route towards creating device structures with more traditional semiconductor nanofabrication techniques.
We present a general picture of the exciton properties of layered materials in terms of the excitations of their single-layer building blocks. To this end, we derive a model excitonic hamiltonian by drawing an analogy with molecular crystals, which are other prototypical van der Waals materials. We employ this simplified model to analyse in detail the excitation spectrum of hexagonal boron nitride (hBN) that we have obtained from the {it ab initio} solution of the many-body Bethe-Salpeter equation as a function of momentum. In this way we identify the character of the lowest-energy excitons in hBN, discuss the effects of the interlayer hopping and the electron-hole exchange interaction on the exciton dispersion, and illustrate the relation between exciton and plasmon excitations in layered materials.
The magnetic excitations in CoPS$_3$, a two-dimensional van der Waals (vdW) antiferromagnet with spin $S=3/2$ on a honeycomb lattice, has been measured using powder inelastic neutron scattering. Clear dispersive spin waves are observed with a large spin gap of ~13 meV. The magnon spectra were fitted using an $XXZ$-type $J_1-J_2-J_3$ Heisenberg Hamiltonian with a single-ion anisotropy assuming no magnetic exchange between the honeycomb layers. The best-fit parameters show ferromagnetic exchange $J_1=-2.08$ meV and $J_2=-0.26$ meV for the nearest and second-nearest neighbors and a sizeable antiferromagnetic exchange $J_3=4.21$ meV for the third-nearest neighbor with the strong easy-axis anisotropy $K=-2.06$ meV. The suitable fitting could only be achieved by the anisotropic $XXZ$-type Hamiltonian, in which the exchange interaction for the out-of-plane component is smaller than that for the in-plane one by a ratio $alpha=J_z/J_x=0.6$. Moreover, the absence of spin-orbit exciton around 30 meV indicates that Co$^{2+}$ ions in CoPS$_3$ have a $S=3/2$ state rather than a spin-orbital entangled $J_rm{eff}=1/2$ ground state. Our result directly shows that CoPS$_3$ is an experimental realization of the $XXZ$ model with a honeycomb lattice in 2D vdW magnets.
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