Atomic Interface Engineering in Two-Dimensional Materials: A Pathway to High-Performance Flexible Thermoelectrics.

The fascinating two-dimensional (2D) materials are being unconsciously applied in various fields from science to engineering, which is benefited from the glamorous physical and chemical properties of mechanics, optics, electronics, and magnetism. The representative 2D thermoelectric/piezoelectric materials can directly convert thermal/mechanical energy into electrical energy, which can resolve the energy issues and avoid further environmental deterioration. The thermoelectric or piezoelectric properties of various 2D materials, such as graphene, hexagonal boron nitride, black phosphorus, transition metal dichalcogenides (TMDs), arsenene, metal carbides and nitrides (MXenes), and so on, have been investigated in detail. Although tremendous progress has been achieved in the past few years, these properties still need to be improved for their practical application by designing new 2D materials, strain engineering, chemical functionalization, etc. In addition to this, in 2D materials, there are many other novel physical properties, such as magnetism, topology, valley, and so on. The combination of thermoelectricity/piezoelectricity with other unique properties may lead to novel device applications or scientific breakthroughs in new physics. Overall, the emergence of 2D thermoelectric and piezoelectric materials has expanded energy conversion research dramatically. By combing this new device concept with the novel 2D materials, original devices should have potential applications in energy harvesting.

A systematic review on 2D materials for volatile organic compound sensing

The isolation of graphene has sparked an unprecedented world wide research activity on the topic of two-dimensional (2D) materials. However, even though graphene has a high potential for various applications, its metallic character is a significant limitation for a large variety of electron devices, starting with the conventional field effect transistor. This limitation could be overcome in the near future by the use of layered van der Waals crystals such as black phosphorus (i.e., phosphorene, which is one to few layers of black phosphorus) and also by other semiconducting 2D materials such as transition metal dichalcogenides (TMDCs) of general formula MX2, where M is the metal and X the chalcogen (S, Se and Te). For instance, phosphorene exhibits a direct band gap varying between ~ 0.3 eV for bulk crystals to ~ 2 eV for a monolayer. In layered TMDC structures, each layer typically comprises 3 atomic planes (corresponding to a thickness below 8 Å), and consists of an hexagonally-organized atomic layer of metal atoms sandwiched between two planes of chalcogen atoms, also in hexagonal configurations. M–X bonds inside each layer are covalent; however, the sandwiching chalcogen layers are linked by weak van der Waals bonds, so that a bulk crystal is easy to cleave along the chalcogen planes. As with phosphorene, most semiconducting TMDC materials also see their band gap increasing as thickness decreases and they switch from indirect to direct band gap for a monolayer. To date, the most studied semiconductor TMDCs are MoS2 and WS2. Because they are atomically thin, 2D materials are particularly well suited for flexible electronics applications. After a brief description of the major features of phosphorene and TMDCs (crystal structures, relevant electronic properties as a function of thickness …), the talk will highlight recent results concerning field effect transistor characteristics. In particular, carrier mobility values as high as 5000 cm2/Vs have been measured in phosphorene films. Since local substitutional-type doping cannot be used in 2D materials, there is a general contacting problem (Schottky barrier formation), which is of paramount importance for device applications. In particular, two types of contacts can be formed: the top contact and the edge contact, which behave differently. Generally speaking, the semiconductor thickness is much smaller than the depletion length at the contact, which is an intriguing and novel situation. In the second part of the talk, various synthesis methods will be presented and discussed, particularly in view of their possible use in the field of large area electronics. For most devices fabricated so far, the 2D layers were obtained by exfoliation of bulk crystals. However, recent progress in synthesis include molecular beam epitaxy, controlled chemical vapour deposition and vapour phase transport. Those various approaches will be discussed, as well as the newly-introduced atomic layer deposition (ALD) process. As most 2D materials are grown on a separate substrate, the transfer problem will be highlighted, particularly concerning phosphorene which is highly hygroscopic, and sensitive to the presence of light. The presentation will be concluded by some perspectives concerning the industrialization of 2D materials.

Recently, black phosphorus (BP), an emerging layered two-dimensional (2D) material, has aroused much research interest. Distinguished from most of other 2D materials, BP is always a direct bandgap semiconductor regardless of the thickness, with the bandgap ranging from 0.3 eV (bulk) to 1.7 eV (monolayer), which is just fill the gap in the bandgap between graphene and transition metal dichalcogenides (TMDCs) in this frequency range. Besides, the BP exhibits many intriguing properties, such as high carrier mobility, highly tunable and anisotropic physical properties, which render the BP another star 2D material following graphene and TMDCs. In this review, we mainly focus on the advances in the optical properties of 2D BP, with the content covering the intrinsic optical properties and external perturbation effects on optical properties. Regarding the intrinsic optical properties, we introduce the anisotropic and layer-dependent optical absorption from interband transitions, the layer-dependent exciton binding energy and exciton absorption, visible-to-infrared photoluminescence, and stability of absorption and photoluminescence. As for external perturbation effects on optical properties, we introduce in-plane uniaxial and biaxial strain effects, gate-induced quantum confined Franz-Keldysh effect and Burstein-Moss effect. And finally we give a brief summary and outlook, pointing out some several interesting and important issues of BP, which need further studying urgently such as hyperbolic plasmons, intersubband transitions, optical properties in heterostructures and twist angle moiré superlattice and so on. This review gives an overview of the optical properties of BP and is expected to arouse the interest in further studying the BP.

The discovery of graphene and its fascinating capabilities has triggered an unprecedented interest in inorganic two-dimensional (2D) materials. van der Waals layered materials such as graphene, hexagonal boron nitride, transition metal dichalcogenides, and the more recently re-discovered black phosphorus (BP) indeed display an exceptional technological potential for engineering nano-electronic and nano-photonic devices and components “by design,” offering a unique platform for developing new devices with a variety of “ad hoc” properties. In this Perspective article, we provide a vision on the key transformative applications of 2D nanomaterials for the development of nanoelectronic, nanophotonic, optical, and plasmonic devices at terahertz frequencies, highlighting how the rich physical phenomena enabled by their unique band structure engineering can allow them to boost the vibrant field of quantum science and quantum technologies.

2D Materials towards sensing technology: From fundamentals to applications

Two-dimensional (2D) materials are crystals with one to a few layers of atoms and are being used in many fields such as optical modulator, photodetector, optical switch, and ultrafast lasers. Their exceptional optoelectronic and nonlinear optical properties make them as a suitable saturable absorber for laser cavities. This review focuses on the recent progress in ultrafast laser use 2D materials as a saturable absorber. 2D materials traditionally include graphene, topological insulators, transition metal dichalcogenides, as well as new materials such as black phosphorus, bismuthene, antimonene, and MXene. Material characteristics, fabrication techniques, and nonlinear properties are also introduced. Finally, future perspectives of ultrafast lasers based on 2D materials are also addressed.

Two-dimensional (2D) materials have captured the attention of the scientific community due to the wide range of unique properties at nanometer-scale thicknesses. While significant exploratory research in 2D materials has been achieved, the understanding of 2D electronic transport and carrier dynamics remains in a nascent stage. Furthermore, because prior review articles have provided general overviews of 2D materials or specifically focused on charge transport in graphene, here we instead highlight charge transport mechanisms in post-graphene 2D materials, with particular emphasis on transition metal dichalcogenides and black phosphorus. For these systems, we delineate the intricacies of electronic transport, including band structure control with thickness and external fields, valley polarization, scattering mechanisms, electrical contacts, and doping. In addition, electronic interactions between 2D materials are considered in the form of van der Waals heterojunctions and composite films. This review concludes with a perspective on the most promising future directions in this fast-evolving field.

Two-dimensional (2D) Van der Waals materials have emerged as a very attractive class of optoelectronic material due to the unprecedented strength in its interaction with light. In this talk I will discuss approaches to enhance and control this interaction by integrating these 2D materials with microcavities, and metamaterials. I will first discuss the formation of strongly coupled half-light half-matter quasiparticles (microcavity excitonpolaritons) [1], their spin-optic [2], and electrical control/excitation (Fig. 1) [3], in the 2D transition metal dichalcogenide (TMD) systems. Prospects for enhanced nonlinear optical interaction using Rydberg states in TMDs will be discussed. Use of photonic hypercrystals and hyperbolic media to enhance the spontaneous emission from the TMDs will also be presented. Following this, I will discuss the routing of valley excitons in 2D TMDs using chiral metasurfaces (Fig. 2) [4]. Finally, time permitting, I will briefly talk about developing deterministic quantum emitters at room temperature using defects in hexagonal boron nitride [5] and prospects of coupling these emitters to high Q resonators.

Different 2D materials that include a wonder material graphene and transition metal dichalcogenides, graphitic carbon nitride (g-C3N4), hexagonal boron nitride (h-BN), and black phosphorus (BP) etc. have been developed with different morphologies and used for gas sensing applications. Work is still going on to improve the sensing capabilities of these materials and their selectivity toward different gases is also being improved using modifiers and filters. For sensing hydrogen, the selectivity of the sensor is also of utmost importance. The selectivity of the sensor can be increased by using the Pt group metals, especially Palladium. Since palladium is a very expensive metal, it is not feasible to use it standalone as a hydrogen gas sensor, rather we can deposit the layer of palladium nanoparticles on the 2D material using physical or chemical method to increase its selectivity for hydrogen sensing. Palladium’s unique ability to form palladium hydride on adsorption of H2 gas molecules by dissociating them into hydrogen atoms and allowing them to move to the sensing layer underneath. In his chapter, we will study the basics of 2D nanomaterials, mechanism of H2 gas sensing, and the advantages of using Pd as a modifier and different polymers as filter.

The scalable preparation of high‐quality and low‐cost two‐dimensional (2D) materials is critical to achieving their potential applications in various fields. Chemical vapor deposition (CVD) method is considered the most promising method for producing ultrathin 2D materials and has continued to develop in recent years. First‐principles calculations have provided important theoretical guidance for the CVD synthesis of 2D materials, and have played an increasingly important role in the field of material synthesis in recent years. In this review, we present recent advances in the growth mechanism of 2D materials, focusing on the theoretical research progress of four typical 2D materials: graphene, hexagonal boron nitride (hBN), transition metal dichalcogenide (TMDC), and phosphorene. Several aspects of the growth process are discussed in detail, including the decomposition of precursors, nucleation, growth kinetics, domain shape, and epitaxial and alignment of 2D crystals. Based on the understanding of these atomic‐scale growth processes, strategies toward the wafer‐scale growth of continuous and homogeneous 2D thin films are proposed and confirmed by experiments. In the final section, we summarize future challenges and opportunities in the computational studies of the growth mechanism of 2D materials.This article is categorized under: Structure and Mechanism > Computational Materials Science Electronic Structure Theory > Density Functional Theory Theoretical and Physical Chemistry > Reaction Dynamics and Kinetics

Direct liquid-phase exfoliation of layered materials by means of ultrasound, shear forces or electrochemical intercalation holds enormous promise as a convenient, cost-effective approach to the mass production of two-dimensional (2D) materials, particularly in the form of colloidal suspensions of high quality and micrometer- and submicrometer-sized flakes. Of special relevance due to environmental and practical reasons is the production of 2D materials in aqueous medium, which generally requires the use of certain additives (surfactants and other types of dispersants) to assist in the exfoliation and colloidal stabilization processes. In this context, biomolecules have received, in recent years, increasing attention as dispersants for 2D materials, as they provide a number of advantages over more conventional, synthetic surfactants. Here, we review research progress in the use of biomolecules as exfoliating and dispersing agents for the production of 2D materials. Although most efforts in this area have focused on graphene, significant advances have also been reported with transition metal dichalcogenides (MoS2, WS2, etc.) or hexagonal boron nitride. Particular emphasis is placed on the specific merits of different types of biomolecules, including proteins and peptides, nucleotides and nucleic acids (RNA, DNA), polysaccharides, plant extracts and bile salts, on their role as efficient colloidal dispersants of 2D materials, as well as on the potential applications that have been explored for such biomolecule-exfoliated materials. These applications are wide-ranging and encompass the fields of biomedicine (photothermal and photodynamic therapy, bioimaging, biosensing, etc.), energy storage (Li- and Na-ion batteries), catalysis (e.g., catalyst supports for the oxygen reduction reaction or electrocatalysts for the hydrogen evolution reaction), or composite materials. As an incipient area of research, a number of knowledge gaps, unresolved issues and novel future directions remain to be addressed for biomolecule-exfoliated 2D materials, which will be discussed in the last part of this review.

Black phosphorus (bP) is a promising two-dimensional (2D) material for opto-electronic applications. Strongly bound excitons with binding energies up to 0.3 eV and remarkably large trion binding energies up to 100 meV have been observed for supported monolayer bP. Surprisingly, this trion binding energy is significantly larger than those found in other 2D materials (e.g. about 30 meV in transition metal dichalcogenides). This has previously been ascribed to the quasi-1D nature of bP. In this work we show, using first principles calculations, that the trion binding energy of bP is indeed large (80 meV) when referenced to the lowest bright exciton but only 30 meV when its energy is measured relative to the lowest dark exciton. Our analysis thus shows that the trion binding energy in bP is not larger than in other 2D materials, and the previous conclusions have to be understood incorporating the large splitting between the dark and bright excitons in bP. We also explore the effect of substrate and in-plane strain of the exciton and trion binding energies and show that these effects do not change the main conclusions. Our results correct the misconception that trion binding energies in monolayer bP are particularly large due to its quasi-1D structure and contribute to the establishment of more a detailed understanding of optical properties of atomically thin semiconductors.

The rapid evolution of wearable and portable electronics has driven an unprecedented demand for flexible, efficient, and durable energy storage solutions. Two-dimensional (2D) materials have captured significant interest due to their unique physical, chemical, and electrochemical characteristics and their ability to create heterostructures with other nanomaterials, enhancing both mechanical strength and electrochemical performance. This chapter delves into the current state-of-the-art knowledge surrounding these advanced flexible 2D material-based flexible lithium-ion batteries (LIBs), highlighting the unique properties of 2D materials that make them ideal for flexible energy storage systems. 2D materials, such as graphene, transition metal dichalcogenides (TMDs), MXenes, and black phosphorus (BP), exhibit exceptional electrical conductivity, large surface area, and mechanical flexibility, and are discussed here. These properties enable the fabrication of LIBs, which offer high energy and power densities and maintain performance under mechanical deformation. This chapter begins with an overview of 2D materials and then delves into recent advancements in 2D material-based flexible LIBs utilizing these materials. There is an emphasis on intricate relationships between the structure and properties of flexible electrodes, particularly focusing on their role in free-standing films. The chapter highlights the integration of these 2D materials into flexible architectures, such as fiber-based devices and wearable electronics, with the potential to revolutionize energy storage by enabling lightweight, flexible, and high-performance devices that conform to various shapes and applications. Fabrication techniques, including inkjet printing, chemical vapor deposition (CVD), and layer-by-layer assembly, facilitate the precise engineering of 2D material-based electrodes and flexible substrates. This chapter addresses the origins of quantum capacitance ( CQ ), its contribution to boosting overall capacitance, and various strategies to enhance CQ . It also reviews the current advancements in CQ for electrode materials, including carbon, 2D materials, and their composites. The concluding section addresses the existing challenges and the prospects for research on flexible LIB devices.

In this review, we survey the recent advances in nonlinear optics and the applications of two‐dimensional (2D) materials. We briefly cover the key developments pertaining to research in the nonlinear optics of graphene, the quintessential 2D material. Subsequently, we discuss the linear and nonlinear optical properties of several other 2D layered materials, including transition metal chalcogenides, black phosphorus, hexagonal boron nitride, perovskites, and topological insulators, as well as the recent progress in hybrid nanostructures containing 2D materials, such as composites with dyes, plasmonic particles, 2D crystals, and silicon integrated structures. Finally, we highlight a few representative current applications of 2D materials to photonic and optoelectronic devices.