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Register a new userFabrication and Imaging of Monolayer Phosphorene with Preferred Edge Configurations via Graphene-Assisted Layer-by-Layer Thinning
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Phosphorene, a monolayer of black phosphorus (BP), is an elemental two-dimensional material with interesting physical properties, such as high charge carrier mobility and exotic anisotropic in-plane properties. To fundamentally understand these various physical properties, it is critically important to conduct an atomic-scale structural investigation of phosphorene, particularly regarding various defects and preferred edge configurations. However, it has been challenging to investigate mono- and few-layer phosphorene because of technical difficulties arising in the preparation of a high-quality sample and damages induced during the characterization process. Here, we successfully fabricate high-quality monolayer phosphorene using a controlled thinning process with transmission electron microscopy, and subsequently perform atomic-resolution imaging. Graphene protection suppresses the e-beam-induced damage to multi-layer BP and one-side graphene protection facilitates the layer-by-layer thinning of the samples, rendering high-quality monolayer and bilayer regions. We also observe the formation of atomic-scale crystalline edges predominantly aligned along the zigzag and (101) terminations, which is originated from edge kinetics under e-beam-induced sputtering process. Our study demonstrates a new method to image and precisely manipulate the thickness and edge configurations of air-sensitive two-dimensional materials.
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There have been continuous efforts to seek for novel functional two-dimensional semiconductors with high performance for future applications in nanoelectronics and optoelectronics. In this work, we introduce a successful experimental approach to fabricate monolayer phosphorene by mechanical cleavage and the following Ar+ plasma thinning process. The thickness of phosphorene is unambiguously determined by optical contrast combined with atomic force microscope (AFM). Raman spectroscopy is used to characterize the pristine and plasma-treated samples. The Raman frequency of A2g mode stiffens, and the intensity ratio of A2g to A1g modes shows monotonic discrete increase with the decrease of phosphorene thickness down to monolayer. All those phenomena can be used to identify the thickness of this novel two-dimensional semiconductor efficiently. This work for monolayer phosphorene fabrication and thickness determination will facilitates the research of phosphorene.
We report on the observation of edge electric currents excited in bi-layer graphene by terahertz laser radiation. We show that the current generation belongs to the class of second order in electric field phenomena and is controlled by the orientation of the THz electric field polarization plane. Additionally, applying a small magnetic field normal to the graphene plane leads to a phase shift in the polarization dependence. Increasing the magnetic field strength, the current starts to exhibit 1/B-magnetooscillations with a period consistent with that of the Shubnikov-de-Haas effect and amplitude by an order of magnitude larger as compared to the current at zero magnetic field measured under the same conditions. The microscopic theory developed shows that the current is formed in the edges vicinity limited by the mean-free path of carriers and the screening length of the high-frequency electric field. The current originates from the alignment of the free carrier momenta and dynamic accumulation of charge at the edges, where the P-symmetry is naturally broken. The observed magnetooscillations of the photocurrent are attributed to the formation of Landau levels.
We performed density functional theory calculations with self-consistent van der Waals corrected exchange-correlation (XC) functionals to capture the structure of black phosphorus and twelve monochalcogenide monolayers and find the following results: (a) The in-plane unit cell changes its area in going from the bulk to a monolayer. The change of in-plane distances implies that bonds weaker than covalent or ionic ones are at work within the monolayers themselves. This observation is relevant for the prediction of the critical temperature $T_c$. (b) There is a hierarchy of independent parameters that uniquely define a ground state ferroelectric unit cell (and square and rectangular paraelectric unit cells as well): only 5 optimizable parameters are needed to establish the unit cell vectors and the four basis vectors of the ferroelectric ground state unit cell, while square and rectangular paraelectric structures are defined by only 3 or 2 independent optimizable variables, respectively. (c) The reduced number of independent structural variables correlates with larger elastic energy barriers on a rectangular paraelectric unit cell when compared to the elastic energy barrier of a square paraelectric structure. This implies that $T_c$ obtained on a structure that keeps the lattice parameters fixed (for example, using an NVT ensemble) should be larger than the transition temperature on a structure that is allowed to change in-plane lattice vectors (for example, using the NPT ensemble). (d) The dissociation energy (bulk cleavage energy) of these materials is similar to the energy required to exfoliate graphite and MoS$_2$. (e) There exists a linear relation among the square paraelectric unit cell lattice parameter and the lattice parameters of the rectangular ferroelectric ground state unit cell. These results highlight the subtle atomistic structure of these novel 2D ferroelectrics.
Black phosphorus (BP) has recently emerged as an alternative 2D semiconductor owing to its fascinating electronic properties such as tunable bandgap and high charge carrier mobility. The structural investigation of few-layer BP, such as identification of layer thickness and atomic-scale edge structure, is of great importance to fully understand its electronic and optical properties. Here we report atomic-scale analysis of few-layered BP performed by aberration corrected transmission electron microscopy (TEM). We establish the layer-number-dependent atomic resolution imaging of few-layer BP via TEM imaging and image simulations. The structural modification induced by the electron beam leads to revelation of crystalline edge and formation of BP nanoribbons. Atomic resolution imaging of BP clearly shows the reconstructed zigzag (ZZ) edge structures, which is also corroborated by van der Waals first principles calculations on the edge stability. Our study on the precise identification of BP thickness and atomic-resolution imaging of edge structures will lay the groundwork for investigation of few-layer BP, especially BP in nanostructured forms.
We consider confinement of Dirac fermions in $AB$-stacked bilayer graphene by inhomogeneous on-site interactions, (pseudo-)magnetic field or inter-layer interaction. Working within the framework of four-band approximation, we focus on the systems where the stationary equation is reducible into two stationary equations with $2times2$ Dirac-type Hamiltonians and auxiliary interactions. We show that it is possible to find localized states by solving an effective Schrodinger equation with energy-dependent potential. We consider several scenarios where bilayer graphene is subject to inhomogneous (pseudo-)magnetic field, on-site interactions or inter-layer coupling. In explicit examples, we provide analytical solutions for the states localized by local fluctuations or periodicity defects of the interactions.
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