Ultrathin two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have attracted considerable attention owing to their unique properties and great potential in a wide range of applications. Great efforts have been devoted to the preparation of novel-structured TMD nanosheets by engineering their intrinsic structures at the atomic scale. Until now, a lot of new-structured TMD nanosheets, such as vacancy-containing TMDs, heteroatom-doped TMDs, TMD alloys, 1T′/1T phase and in-plane TMD crystal-phase heterostructures, TMD heterostructures and Janus TMD nanosheets, have been prepared. These materials exhibit unique properties and hold great promise in various applications, including electronics/optoelectronics, thermoelectrics, catalysis, energy storage and conversion and biomedicine. This review focuses on the most recent important discoveries in the preparation, characterization and application of these new-structured ultrathin 2D layered TMDs.

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Novel structured transition metal dichalcogenide nanosheets

Ever since the isolation of single-layer graphene in 2004, two-dimensional layered structures have been among the most extensively studied classes of materials. To date, the pool of two-dimensional materials (2DMs) continues to grow at an accelerated pace and already covers an extensive range of fascinating and technologically relevant properties. An array of experimental techniques have been developed and used to characterize and understand these properties. In particular, Raman spectroscopy has proven to be a key experimental technique, thanks to its capability to identify minute structural and electronic effects in nondestructive measurements. While high-frequency (HF) intralayer Raman modes have been extensively employed for 2DMs, recent experimental and theoretical progress has demonstrated that low-frequency (LF) interlayer Raman modes are more effective at determining layer numbers and stacking configurations and provide a unique opportunity to study interlayer coupling. These advantages are due to...

Low-Frequency Shear and Layer-Breathing Modes in Raman Scattering of Two-Dimensional Materials.

Recently, charge-density wave (CDW) and superconductivity are observed to coexist in atomically thin metallic NbSe2. Lacking of knowledge on the structural details of CDW, however, prevents us to explore its interplay with superconductivity. Using first-principles calculations, we identify the ground state 3 × 3 CDW atomic structure of monolayer NbSe2, which is characterized by the formation of triangular Nb clusters and shows a scanning tunnelling microscopy (STM) image and Raman CDW modes in good agreement with experiments. We further demonstrate that from bulk to monolayer NbSe2, as the layer thickness decreases, the CDW order is gradually enhanced with rising energy gain and strengthened Fermi surface gapping, while superconductivity is weakened due to the increasingly reduced Fermi level density of states in the CDW state. These results well explain the observed opposite thickness dependencies of CDW and superconducting transition temperatures and uncover the nature of competitive interaction between...

Unveiling Charge-Density Wave, Superconductivity, and Their Competitive Nature in Two-Dimensional NbSe2

In this work, we show unusual effects of strong interlayer coupling on low-frequency (LF) Raman scattering in exfoliated PdSe2 crystals with different number of layers. Unlike many other layered materials, it is found that the measured frequencies of the breathing modes cannot be simply described by a conventional linear chain model (LCM) that treats each layer as a single rigid object. By using first-principles calculations, we show that strong deviations from layer rigidity can occur for the LF breathing vibrations of PdSe2, which accounts for the observed disagreement with the conventional LCM. The layer non-rigidity and strong interlayer coupling could also explain the unusual strong intensities of the LF breathing modes that are comparable with those of the high-frequency Raman modes. These strong intensities allowed us to use a set of the measured LF Raman lines as unique fingerprints for a precise assignment of the layer numbers. The assignment of the layer numbers was further confirmed using second harmonic generation that appeared only in the noncentrosymmetric even-layer PdSe2 crystals. This work thus demonstrates a simple and fast approach for the determination of the number of layers in 2D materials with strong interlayer coupling and non-rigid interlayer vibrations.

http://iopscience.iop.org/article/10.1088/2053-1583/aabe4d/pdf

Anomalous interlayer vibrations in strongly coupled layered PdSe 2

Atomically thin two-dimensional (2D) materials exhibit enormous potential in photodetectors because of novel and extraordinary properties, such as passivated surfaces, tunable bandgaps, and high mobility. High-performance photodetectors based on 2D materials have been fabricated for broadband, position, polarization-sensitive detection, and large-area array imaging. However, the current performance of 2D material photodetectors is not outstanding enough, including response speed, detectivity, and so forth. The way to further promote the development of 2D material photodetectors and their corresponding practical applications is still a tremendous challenge. In this article, these issues of 2D material photodetectors are analyzed and expected to be solved by combining micro-nano characterization technologies. The inherent physical properties of 2D materials and photodetectors can be accurately characterized by Raman spectroscopy, transmission electron microscopy (TEM), and scattering scanning near-field optical microscope (s-SNOM). In particular, the precise probe of lattice defects, doping concentration, and near-field light absorption characteristics can promote the researches of low-noise and high-responsivity photodetectors. Scanning photocurrent microscope (SPCM) can show the overall spatial distribution of photocurrent and analyze the mechanism of photocurrent. Photoluminescence (PL) spectroscopy and Kelvin probe force microscope (KPFM) can characterize the material bandgap, work function distribution and interlayer coupling characteristics, making it possible to design high-performance photodetectors through energy band engineering. These advanced characterization techniques cover the entire process from material growth, to device preparation, and to performance analysis, and systematically reveal the development status of 2D material photodetectors. Finally, the prospects and challenges are discussed to promote the application of 2D material photodetectors.

Recent progress and challenges on two-dimensional material photodetectors from the perspective of advanced characterization technologies

Atomically thin NbSe2 is a metallic layered transition metal dichalcogenide with novel charge-density-wave (CDW) and superconductive phases. Properties of NbSe2 atomic layers are sensitive to interlayer coupling. Here we investigate the interlayer phonons of few-layer NbSe2 by ultralow-frequency Raman spectroscopy. We observe both the interlayer breathing modes and shear modes at frequencies below 40 cm−1 for samples of 2–15 layers. Their frequency, Raman activity, and environmental instability depend systematically on the layer number. We account for these results by a combination of linear-chain model, group theory and first-principles calculations. We find that, although NbSe2 has different stacking order from MoS2, MoSe2, WS2 and WSe2, they share the same crystal symmetry groups and exhibit similar Raman selection rules for interlayer phonons. In addition, the interlayer phonon modes evolve smoothly from T = 300 to 8 K, with no observable response to the CDW formation in NbSe2. This finding indicates that the atomic registry between adjacent NbSe2 layers is well preserved in the CDW transition.

https://iopscience.iop.org/article/10.1088/2053-1583/3/3/031008/pdf

Interlayer breathing and shear modes in NbSe2 atomic layers

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Interlayer breathing and shear modes in NbSe2 atomic layers