Ultrathin Two‐Dimensional Multinary Layered Metal Chalcogenide Nanomaterials

Ultrathin two‐dimensional (2D) layered transition metal dichalcogenides (TMDs), such as MoS₂, WS₂, TiS₂, TaS₂, ReS₂, MoSe₂ and WSe₂, have attracted considerable attention over the past six years owing to their unique properties and great potential in a wide range of applications. Aiming to achieve tunable properties and optimal application performances, great effort is devoted to the exploration of 2D multinary layered metal chalcogenide nanomaterials, which include ternary metal chalcogenides with well‐defined crystal structures, alloyed TMDs, heteroatom‐doped TMDs and 2D metal chalcogenide heteronanostructures. These novel 2D multinary layered metal chalcogenide nanomaterials exhibit some unique properties compared to 2D binary TMD counterparts, thus holding great promise in various potential applications including electronics/optoelectronics, catalysis, sensors, biomedicine, and energy storage and conversion with enhanced performances. This article focuses on the state‐of‐art progress on the preparation, characterization and applications of ultrathin 2D multinary layered metal chalcogenide nanomaterials.     

Exotic Magnetic Anisotropy Near Digitized Dimensional Mott Boundary

The magnetic anisotropy of low-dimensional Mott systems exhibits unexpected magnetotransport behavior useful for spin-based quantum electronics. Yet, the anisotropy of natural materials is inherently determined by the crystal structure, highly limiting its engineering. The magnetic anisotropy modulation near a digitized dimensional Mott boundary in artificial superlattices composed of a correlated magnetic monolayer SrRuO₃ and nonmagnetic SrTiO₃, is demonstrated. The magnetic anisotropy is initially engineered by modulating the interlayer coupling strength between the magnetic monolayers. Interestingly, when the interlayer coupling strength is maximized, a nearly degenerate state is realized, in which the anisotropic magnetotransport is strongly influenced by both the thermal and magnetic energy scales. The results offer a new digitized control for magnetic anisotropy in low-dimensional Mott systems, inspiring promising integration of Mottronics and spintronics.     

Two‐Dimensional Arrays of Transition Metal Nitride Nanocrystals

The synthesis of low‐dimensional transition metal nitride (TMN) nanomaterials is developing rapidly, as their fundamental properties, such as high electrical conductivity, lead to many important applications. However, TMN nanostructures synthesized by traditional strategies do not allow for maximum conductivity and accessibility of active sites simultaneously, which is a crucial factor for many applications in plasmonics, energy storage, sensing, and so on. Unique interconnected two‐dimensional (2D) arrays of few‐nanometer TMN nanocrystals not only having electronic conductivity in‐plane, but also allowing transport of ions and electrolyte through the porous nanosheets, which are obtained by topochemical synthesis on the surface of a salt template, are reported. As a demonstration of their application in a lithium–sulfur battery, it is shown that 2D arrays of several nitrides can achieve a high initial capacity of >1000 mAh g^?1 at 0.2 C and only about 13% degradation over 1000 cycles at 1 C under a high areal sulfur loading (>5 mg cm^?2).     

Scalable Design of Two‐Dimensional Oxide Nanosheets for Construction of Ultrathin Multilayer Nanocapacitor

Large size of capacitors is the main hurdle in miniaturization of current electronic devices. Herein, a scalable solution‐based layer‐by‐layer engineering of metallic and high‐κ dielectric nanosheets into multilayer nanosheet capacitors (MNCs) with overall thickness of ≈20 nm is presented. The MNCs are built through neat tiling of 2D metallic Ru_0.95O₂^0.2? and high‐κ dielectric Ca₂NaNb₄O₁₃^? nanosheets via the Langmuir–Blodgett (LB) approach at room temperature which is verified by cross‐sectional high‐resolution transmission electron microscopy (HRTEM). The resultant MNCs demonstrate a high capacitance of 40–52 µF cm^?2 and low leakage currents down to 10^?5–10^?6 A cm^?2. Such MNCs also possess complimentary in situ robust dielectric properties under high‐temperature measurements up to 250 °C. Based on capacitance normalized by the thickness, the developed MNC outperforms state‐of‐the‐art multilayer ceramic capacitors (MLCC, ≈22 µF cm^?2/5 × 10⁴ nm) present in the market. The strategy is effective due to the advantages of facile, economical, and ambient temperature solution assembly.     

Low‐Dimensional Topological Crystalline Insulators

Topological crystalline insulators (TCIs) are recently discovered topological phase with robust surface states residing on high‐symmetry crystal surfaces. Different from conventional topological insulators (TIs), protection of surface states on TCIs comes from point‐group symmetry instead of time‐reversal symmetry in TIs. The distinct properties of TCIs make them promising candidates for the use in novel spintronics, low‐dissipation quantum computation, tunable pressure sensor, mid‐infrared detector, and thermoelectric conversion. However, similar to the situation in TIs, the surface states are always suppressed by bulk carriers, impeding the exploitation of topology‐induced quantum phenomenon. One effective way to solve this problem is to grow low‐dimensional TCIs which possess large surface‐to‐volume ratio, and thus profoundly increase the carrier contribution from topological surface states. Indeed, through persistent effort, researchers have obtained unique quantum transport phenomenon, originating from topological surface states, based on controllable growth of low‐dimensional TCIs. This article gives a comprehensive review on the recent progress of controllable synthesis and topological surface transport of low‐dimensional TCIs. The possible future direction about low‐dimensional TCIs is also briefly discussed at the end of this paper.     

Ramp‐Reversal Memory and Phase‐Boundary Scarring in Transition Metal Oxides

Transition metal oxides are complex electronic systems that exhibit a multitude of collective phenomena. Two archetypal examples are VO₂ and NdNiO₃, which undergo a metal–insulator phase transition (MIT), the origin of which is still under debate. Here this study reports the discovery of a memory effect in both systems, manifested through an increase of resistance at a specific temperature, which is set by reversing the temperature ramp from heating to cooling during the MIT. The characteristics of this ramp‐reversal memory effect do not coincide with any previously reported history or memory effects in manganites, electron‐glass or magnetic systems. From a broad range of experimental features, supported by theoretical modelling, it is found that the main ingredients for the effect to arise are the spatial phase separation of metallic and insulating regions during the MIT and the coupling of lattice strain to the local transition temperature of the phase transition. We conclude that the emergent memory effect originates from phase boundaries at the reversal temperature leaving “scars” in the underlying lattice structure, giving rise to a local increase in the transition temperature. The universality and robustness of the effect shed new light on the MIT in complex oxides.     

25th Anniversary Article: Hybrid Nanostructures Based on Two‐Dimensional Nanomaterials

Two‐dimensional (2D) nanomaterials, such as graphene and transition metal dichalcogenides (TMDs), receive a lot of attention, because of their intriguing properties and wide applications in catalysis, energy‐storage devices, electronics, optoelectronics, and so on. To further enhance the performance of their application, these 2D nanomaterials are hybridized with other functional nanostructures. In this review, the latest studies of 2D nanomaterial‐based hybrid nanostructures are discussed, focusing on their preparation methods, properties, and applications.     

Quantum‐Hall to Insulator Transition in Ultra‐Low‐Carrier‐Density Topological Insulator Films and a Hidden Phase of the Zeroth Landau Level

A key feature of the topological surface state under a magnetic field is the presence of the zeroth Landau level at the zero energy. Nonetheless, it is challenging to probe the zeroth Landau level due to large electron–hole puddles smearing its energy landscape. Here, by developing ultra‐low‐carrier density topological insulator Sb₂Te₃ films, an extreme quantum limit of the topological surface state is reached and a hidden phase at the zeroth Landau level is uncovered. First, an unexpected quantum‐Hall‐to‐insulator‐transition near the zeroth Landau level is discovered. Then, through a detailed scaling analysis, it is found that this quantum‐Hall‐to‐insulator‐transition belongs to a new universality class, implying that the insulating phase discovered here has a fundamentally different origin from those in nontopological systems.     

Solution Processed Metal Oxide High‐κ Dielectrics for Emerging Transistors and Circuits

The electronic functionalities of metal oxides comprise conductors, semiconductors, and insulators. Metal oxides have attracted great interest for construction of large‐area electronics, particularly thin‐film transistors (TFTs), for their high optical transparency, excellent chemical and thermal stability, and mechanical tolerance. High‐permittivity (κ) oxide dielectrics are a key component for achieving low‐voltage and high‐performance TFTs. With the expanding integration of complementary metal oxide semiconductor transistors, the replacement of SiO₂ with high‐κ oxide dielectrics has become urgently required, because their provided thicker layers suppress quantum mechanical tunneling. Toward low‐cost devices, tremendous efforts have been devoted to vacuum‐free, solution processable fabrication, such as spin coating, spray pyrolysis, and printing techniques. This review focuses on recent progress in solution processed high‐κ oxide dielectrics and their applications to emerging TFTs. First, the history, basics, theories, and leakage current mechanisms of high‐κ oxide dielectrics are presented, and the underlying mechanism for mobility enhancement over conventional SiO₂ is outlined. Recent achievements of solution‐processed high‐κ oxide materials and their applications in TFTs are summarized and traditional coating methods and emerging printing techniques are introduced. Finally, low temperature approaches, e.g., ecofriendly water‐induced, self‐combustion reaction, and energy‐assisted post treatments, for the realization of flexible electronics and circuits are discussed.     

N‐Type Superconductivity in an Organic Mott Insulator Induced by Light‐Driven Electron‐Doping

The presence of interface dipoles in self‐assembled monolayers (SAMs) gives rise to electric‐field effects at the device interfaces. SAMs of spiropyran derivatives can be used as photoactive interface dipole layer in field‐effect transistors because the photochromism of spiropyrans involves a large dipole moment switching. Recently, light‐induced p‐type superconductivity in an organic Mott insulator, κ‐(BEDT‐TTF)₂Cu[N(CN)₂]Br (κ‐Br: BEDT‐TTF = bis(ethylenedithio)tetrathiafulvalene) has been realized, thanks to the hole carriers induced by significant interface dipole variation in the spiropyran‐SAM. This report explores the converse situation by designing a new type of spiropyran monolayer in which light‐induced electron‐doping into κ‐Br and accompanying n‐type superconducting transition have been observed. These results open new possibilities for novel electronics utilizing a photoactive SAMs, which can design not only the magnitude but also the direction of photoinduced electric‐fields at the device interfaces.     

Exploring Two‐Dimensional Transport Phenomena in Metal Oxide Heterointerfaces for Next‐Generation,High‐Performance,Thin‐Film Transistor Technologies

In the last decade, metal oxides have emerged as a fascinating class of electronic material, exhibiting a wide range of unique and technologically relevant characteristics. For example, thin‐film transistors formed from amorphous or polycrystalline metal oxide semiconductors offer the promise of low‐cost, large‐area, and flexible electronics, exhibiting performances comparable to or in excess of incumbent silicon‐based technologies. Atomically flat interfaces between otherwise insulating or semiconducting complex oxides, are also found to be highly conducting, displaying 2‐dimensional (2D) charge transport properties, strong correlations, and even superconductivity. Field‐effect devices employing such carefully engineered interfaces are hoped to one day compete with traditional group IV or III–V semiconductors for use in the next‐generation of high‐performance electronics. In this Concept article we provide an overview of the different metal oxide transistor technologies and potential future research directions. In particular, we look at the recent reports of multilayer oxide thin‐film transistors and the possibility of 2D electron transport in these disordered/polycrystalline systems and discuss the potential of the technology for applications in large‐area electronics.