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2D materials with phase transitions, such as charge density wave and magnetic and dipole orderings, are an important subfamily of 2D materials. Strong charge–spin–lattice couplings in the materials enable vast potentials for new‐concept and new‐structure devices. Recent experimental progress on the synthesis and device demonstration based 2D phase‐transition materials, such as 1T‐TaS₂, CrI₃, and Cr₂Ge₂Te₆ monolayers, is reviewed.

Abstract

Layered materials with phase transitions, such as charge density wave (CDW) and magnetic and dipole ordering, have potential to be exfoliated into monolayers and few‐layers and then become a large and important subfamily of two‐dimensional (2D) materials. Benefitting from enriched physical properties from the collective interactions, long‐range ordering, and related phase transitions, as well as the atomic thickness yet having nondangling bonds on the surface, 2D phase‐transition materials have vast potential for use in new‐concept and functional devices. Here, potential 2D phase‐transition materials with CDWs and magnetic and dipole ordering, including transition metal dichalcogenides, transition metal halides, metal thio/selenophosphates, chromium silicon/germanium tellurides, and more, are introduced. The structures and experimental phase‐transition properties are summarized for the bulk materials and some of the obtained monolayers. In addition, recent experimental progress on the synthesis and measurement of monolayers, such as 1T‐TaS₂, CrI₃, and Cr₂Ge₂Te₆, is reviewed.

The strain engineering of 2D materials is particularly exciting, because an individual sheet can survive remarkably large mechanical strain and its atomic thinness allows mechanical deformations like a piece of paper. These exceptional circumstances create opportunities for the study of new fundamental physics and applications of 2D materials emerging at the large strain level.

Abstract

Triggered by the growing needs of developing semiconductor devices at ever‐decreasing scales, strain engineering of 2D materials has recently seen a surge of interest. The goal of this principle is to exploit mechanical strain to tune the electronic and photonic performance of 2D materials and to ultimately achieve high‐performance 2D‐material‐based devices. Although strain engineering has been well studied for traditional semiconductor materials and is now routinely used in their manufacturing, recent experiments on strain engineering of 2D materials have shown new opportunities for fundamental physics and exciting applications, along with new challenges, due to the atomic nature of 2D materials. Here, recent advances in the application of mechanical strain into 2D materials are reviewed. These developments are categorized by the deformation modes of the 2D material–substrate system: in‐plane mode and out‐of‐plane mode. Recent state‐of‐the‐art characterization of the interface mechanics for these 2D material–substrate systems is also summarized. These advances highlight how the strain or strain‐coupled applications of 2D materials rely on the interfacial properties, essentially shear and adhesion, and finally offer direct guidelines for deterministic design of mechanical strains into 2D materials for ultrathin semiconductor applications.

The construction of different heterostructures based on 2D materials offers great opportunities for boosting the catalytic activity in electo(photo)chemical reactions. Starting from the theoretical background of the fundamental concepts, the progressive developments in the design and applications of heterostructures based on 2D materials are summarized.

Abstract

The unique structural and electronic properties of 2D materials, including the metal and metal‐free ones, have prompted intense exploration in the search for new catalysts. The construction of different heterostructures based on 2D materials offers great opportunities for boosting the catalytic activity in electo(photo)chemical reactions. Particularly, the merits resulting from the synergism of the constituent components and the fascinating properties at the interface are tremendously interesting. This scenario has now become the state‐of‐the‐art point in the development of active catalysts for assisting energy conversion reactions including water splitting and CO₂ reduction. Here, starting from the theoretical background of the fundamental concepts, the progressive developments in the design and applications of heterostructures based on 2D materials are traced. Furthermore, a personal perspective on the exploration of 2D heterostructures for further potential application in catalysis is offered.

Two-dimensional synthetic polymers (2DSPs) are sheet-like macromolecules consisting of covalently linked repeat units in two directions. Access to 2DSPs with controlled size and shape and diverse functionality has been limited because of the need for monomers to retain their crystallinity throughout polymerization. Here, we describe a synthetic strategy for 2DSPs that obviates the need for crystallinity, via the free radical copolymerization of amphiphilic gemini monomers and their monomeric derivatives arranged in a bilayer at solid-liquid interfaces. The ease of this strategy allowed the preparation of 2DSPs with well-controlled size and shape and diverse functionality on solid templates composed of various materials with wide-ranging surface curvatures and dimensions. The resulting 2DSPs showed remarkable mechanical strength and have multiple applications, such as nanolithographic resist and antibacterial agent. The broad scope of this approach markedly expands the chemistry, morphology, and functionality of 2DSPs accessible for practical applications.

Solid-state thermionic devices based on van der Waals structures were proposed for nanoscale thermal to electrical energy conversion and integrated electronic cooling applications. We study thermionic cooling across gold-graphene-WSe₂-graphene-gold structures computationally and experimentally. Graphene and WSe₂ layers were stacked, followed by deposition of gold contacts. The I-V curve of the structure suggests near-ohmic contact. A hybrid technique that combines thermoreflectance and cooling curve measurements is used to extract the device ZT. The measured Seebeck coefficient, thermal and electrical conductance, and ZT values at room temperatures are in agreement with the theoretical predictions using first-principles calculations combined with real-space Green’s function formalism. This work lays the foundation for development of efficient thermionic devices.

Graphene is a powerful playground for studying a plethora of quantum phenomena. One of the remarkable properties of graphene arises when it is strained in particular geometries and the electrons behave as if they were under the influence of a magnetic field. Previously, these strain-induced pseudomagnetic fields have been explored on the nano- and micrometer-scale using scanning probe and transport measurements. Heteroepitaxial strain, in contrast, is a wafer-scale engineering method. Here, we show that pseudomagnetic fields can be generated in graphene through wafer-scale epitaxial growth. Shallow triangular nanoprisms in the SiC substrate generate strain-induced uniform fields of 41 T, enabling the observation of strain-induced Landau levels at room temperature, as detected by angle-resolved photoemission spectroscopy, and confirmed by model calculations and scanning tunneling microscopy measurements. Our work demonstrates the feasibility of exploiting strain-induced quantum phases in two-dimensional Dirac materials on a wafer-scale platform, opening the field to new applications.

Skin-like sensory devices should be stretchable and self-healable to meet the demands for future electronic skin applications. Despite recent notable advances in skin-inspired electronic materials, it remains challenging to confer these desired functionalities to an active semiconductor. Here, we report a strain-sensitive, stretchable, and autonomously self-healable semiconducting film achieved through blending of a polymer semiconductor and a self-healable elastomer, both of which are dynamically cross-linked by metal coordination. We observed that by controlling the percolation threshold of the polymer semiconductor, the blend film became strain sensitive, with a gauge factor of 5.75 x 10⁵ at 100% strain in a stretchable transistor. The blend film is also highly stretchable (fracture strain, >1300%) and autonomously self-healable at room temperature. We proceed to demonstrate a fully integrated 5 x 5 stretchable active-matrix transistor sensor array capable of detecting strain distribution through surface deformation.

Measuring the behavior of redox-active molecules in space and time is crucial for understanding chemical and biological systems and for developing new technologies. Optical schemes are noninvasive and scalable, but usually have a slow response compared to electrical detection methods. Furthermore, many fluorescent molecules for redox detection degrade in brightness over long exposure times. Here, we show that the photoluminescence of "pixel" arrays of monolayer MoS₂ can image spatial and temporal changes in redox molecule concentration. Because of the strong dependence of MoS₂ photoluminescence on doping, changes in the local chemical potential substantially modulate the photoluminescence of MoS₂, with a sensitivity of 0.9 on a 5 μm x 5 μm pixel, corresponding to better than parts-per-hundred changes in redox molecule concentration down to nanomolar concentrations at 100-ms frame rates. This provides a new strategy for visualizing chemical reactions and biomolecules with a two-dimensional material screen.