Atomically thin layered III–VI metal chalcogenides are an emerging class of 2D materials that have attracted increasing attention in recent years due to their remarkable physical properties and technological applications. Thanks to the recently developed theoretical and experimental methods, a number of exciting discoveries for these materials have revealed their new phases, a unique “Mexican hat”-shaped electronic band structure, and superior optical and electronic properties that distinguish them from other 2D materials such as transition metal dichalcogenides. This review summarizes the novel properties, structures, and synthesis strategies for these materials and emphasizes the most cutting-edge and seminal achievements in this rapidly growing field in order to provide input for future research works. We first present the rich crystal structure and phases that have been found in these materials, with an emphasis on the possibility of phase engineering. Then, we discuss the synthesis strategies for 2D layered III–VI metal chalcogenides from the top-down, bottom-up, and template-based chemical conversion approaches. We focus on the highly controlled synthesis methods that provide fine-tuning of the thickness, phase, edge structure, and other morphological characteristics. Third, we discuss the properties and applications of these materials, focusing on their unique electronic structure including the Mexican hat-shaped valence band, their superior nonlinear optical properties, high-performance electronic devices, promising photoelectrochemical properties, and emerging quantum properties such as quantum emission, exciton condensation, ferromagnetism, and topological quantum phase transition. Finally, we provide our perspective on the current challenges and future directions in this field.

Synthesis and emerging properties of 2D layered III–VI metal chalcogenides

2D metal oxides (2DMOs) have been widely applied in the fields of electronic, magnetic, optical, and catalytic materials, owing to their rich surface chemistry and unique electronic structures. However, their further development faces challenges such as the difficulty in fabricating 2DMOs with unstable surface induced by strong surface polarizability, or the high cost and limited yield of the fabrication process. Recently, liquid metals have shown great potential in the fabrication of 2DMOs. The native oxide skin formed on the surface of liquid metals can be considered as a perfect 2D planar material. Due to the solubility, fluidity, and reactivity of liquid metals, they can act as the solvent, reactant, and interface in the fabrication of 2DMOs. Moreover, liquid metals undergo a liquid-solid phase transition, enabling them to be a symmetric matched substrate for growing high-quality 2DMOs. An insightful survey of the recent progress in this research direction is presented. The features of liquid metals including good solubility, chemical reactivity, weak interface force, and liquid-solid phase transitions are introduced in detail. Furthermore, strategies for the fabrication of 2DMOs by virtue of these features are summarized comprehensively. Finally, current challenges and prospects regarding the future development in the fabrication of 2DMOs via liquid metals are highlighted.

Liquid Metals: A Novel Possibility of Fabricating 2D Metal Oxides

A gas-mediated fabrication of centimeter-scale two-dimensional (2D) semiconductors and ultraviolet photodetector by a liquid metal-based printing was reported. Various large-scale 2D materials (Ga2O3, In2O3, SnO) were demonstrated to be directly printed at ambient air on different substrates. Such printing represents a generic, fast, clean, and scalable technique to quickly manufacture 2D semiconductors. The electrical properties were explored to quantify the printed 2D films, which were somewhat deficient in previous studies. In particular, to explore and facilitate the advantages of this 2D semiconductor in functional electronic applications, strategies for realizing fully printed Ga2O3/Si heterojunction photodetector via low-temperature and low-cost processes were developed. The device exhibits excellent sensibility and rapid photoresponse times. This work offers feasible way to develop high-performance ultraviolet photodetector for mass production. It also suggests a promising direction for making large-scale 2D photoelectronic and electronic systems and is expected to be extensively useful in the coming time.

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Gas-mediated liquid metal printing toward large-scale 2D semiconductors and ultraviolet photodetector

Ultrathin two-dimensional (2D) materials exhibit broad application prospects in many fields due to the enhanced specific surface area to volume ratio and quantum confinement effect. Because of the atomic thickness and various orientations, ultrathin 2D materials exposing specific facets have drawn great attention for various applications in catalysis, batteries, optoelectronics, magnetism, epitaxial template for material growth, etc. Though maintaining the atomic thickness of 2D materials while controlling crystal facets is an enormous challenge, breakthroughs are being made. This review provides a comprehensive overview of the recent advances in the facet engineering of 2D materials, ranging from a basic understanding of facets and the corresponding approaches and the significance of facet engineering. We also propose current challenges and forecast future development directions including the establishment of a facet database, the fabrication of new 2D materials, the design of specific substrates, and the introduction of theoretical calculations and in situ characterization techniques. This review can guide researchers to design ultrathin 2D materials with unique and distinct facets and provide an insight into the applications of energy, magnetism, optics, biomedicine, and other fields.

Facet engineering of ultrathin two-dimensional materials.

Precise Vapor-Phase Synthesis of Two-Dimensional Atomic Single Crystals

Currently, most two-dimensional (2D) materials that are of interest to emergent applications have focused on van der Waals–layered materials (VLMs) because of the ease with which the layers can be ...

/pdf/molecular-scaffold-growth-of-two-dimensional-strong-4x383prdlv.pdf

Molecular Scaffold Growth of Two-Dimensional, Strong Interlayer-Bonding-Layered Materials

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Molecular Scaffold Growth of Two-Dimensional, Strong Interlayer-Bonding-Layered Materials