High-Yield Exfoliation of Stanene Nanodots for High-Performance Organic Light-Emitting Diodes.

Stanene nanodots (SnNDs) derived from layered tin have attracted considerable interest due to their conveniently tunable bandgap and topological superconductivity. However, high-yield exfoliation of ultrathin SnNDs is still a challenge due to the short layer spacing and strong binding energy. In this work, atomically thin SnNDs with a uniform size of 2.3 nm are successfully prepared by utilizing imidazolium ionic liquid-assisted exfoliation. The obtained SnNDs possess a wide bandgap of 2.69 eV, along with notable solvent compatibility (well dispersed in both polar and nonpolar solvents) and excellent stability. Furthermore, we construct Ir(ppy)3-based green OLED with hybridizing SnNDs and graphene oxide (GO) as the hole injection layer (HIL). It proves that the application of SnNDs helps to modulate the work function and passivate surface defects of GO, increasing hole mobility and thereby improving the device performance. Compared to the PEDOT:PSS-based control device, the optimized SnNDs-GO-based OLED demonstrates an improvement of 6.56, 41.06, and 8.16% in current efficiency (CE), power efficiency (PE), and external quantum efficiency (EQE), respectively. This work not only introduces a new approach to preparing 2D SnNDs but also creates a novel HIL material for OLED devices.

Chromium(II)-isophthalate 2D MOF with Redox-Tailorable Gas Adsorption Selectivity.

Redox-active metal-organic frameworks (MOFs) are very promising materials due to their potential capabilities for postsynthetic modification aimed at tailoring their application properties. However, the research field related to redox-active MOFs is still relatively underdeveloped, which limits their practical application. We investigated the self-assembly process of Cr(II) ions and isophthalate (m-bdc) linkers, which have been previously demonstrated to yield 0D metal-organic polyhedra. However, using the diffusion-controlled synthetic approach, we demonstrate the selective preparation of a 2D-layered Cr(II)-based MOF material [Cr(m-bdc)]·H2O (1·H2O). Remarkably, the controlled oxidation of the developed 2D MOF using nitric oxide or dry oxygen resulted in modified porous materials with excellent H2/N2 adsorption selectivities.

2D TMDC aging: a case study of monolayer WS2 and mitigation strategies.

Due to their unique properties, two-dimensional transition metal dichalcogenides (2D TMDCs) are considered for diverse applications in microelectronics, sensing, catalysis, to name a few. A common challenge in 2D TMDC research is the film's inherent instability i.e., spontaneous oxidation upon ambient exposure. The present study systematically explores the effect aging on the film composition and photoluminescent properties of monolayer WS2, synthetically grown by metal-organic chemical vapor deposition. The aging rate is investigated for different oxygen (i.e., O2 gas concentration and humidity) and light-controlled environments. Simple mitigation strategies that do not involve capping the 2D TMDC layer are discussed, and their effectiveness demonstrated by benchmarking the evolution in photoluminescence response against ambient exposed monolayer WS2. These results highlight the need to store 2D TMDCs in controlled environments to preserve the film quality and how future studies can account for the aging effect.

Versatile Method for Preparing Two-Dimensional Metal Dihalides.

Ever since the ground-breaking isolation of graphene, numerous two-dimensional (2D) materials have emerged with 2D metal dihalides gaining significant attention due to their intriguing electrical and magnetic properties. In this study, we introduce an innovative approach via anhydrous solvent-induced recrystallization of bulk powders to obtain crystals of metal dihalides (MX2, with M = Cu, Ni, Co and X = Br, Cl, I), which can be exfoliated to 2D flakes. We demonstrate the effectiveness of our method using CuBr2 as an example, which forms large layered crystals. We investigate the structural properties of both the bulk and 2D CuBr2 using X-ray diffraction, along with Raman scattering and optical spectroscopy, revealing its quasi-1D chain structure, which translates to distinct emission and scattering characteristics. Furthermore, microultraviolet photoemission spectroscopy and electronic transport reveal the electronic properties of CuBr2 flakes, including their valence band structure. We extend our methodology to other metal halides and assess the stability of the metal halide flakes in controlled environments. We show that optical contrast can be used to characterize the flake thicknesses for these materials. Our findings demonstrate the versatility and potential applications of the proposed methodology for preparing and studying 2D metal halide flakes.

Realization of Extremely High-Gain and Low-Power in nMOS Inverter Based on Monolayer WS2 Transistor Operating in Subthreshold Regime.

In this work, we report an n-type metal-oxide-semiconductor (nMOS) inverter using chemical vapor deposition (CVD)-grown monolayer WS2 field-effect transistors (FETs). Our large-area CVD-grown monolayer WS2 FETs exhibit outstanding electrical properties including a high on/off ratio, small subthreshold swing, and excellent drain-induced barrier lowering. These are achieved by n-type doping using AlOx/Al2O3 and a double-gate structure employing high-k dielectric HfO2. Due to the superior subthreshold characteristics, monolayer WS2 FETs show high transconductance and high output resistance in the subthreshold regime, resulting in significantly higher intrinsic gain compared to conventional Si MOSFETs. Therefore, we successfully realize subthreshold operating monolayer WS2 nMOS inverters with extremely high gains of 564 and 2056 at supply voltage (VDD) of 1 and 2 V, respectively, and low power consumption of ∼2.3 pW·µm-1 at VDD = 1 V. In addition, the monolayer WS2 nMOS inverter is further expanded to the demonstration of logic circuits such as AND, OR, NAND, NOR logic gates, and SRAM. These findings suggest the potential of monolayer WS2 for high-gain and low-power logic circuits and validate the practical application in large areas.

Two-Dimensional M-Chalcogene Family with Tunable Superconducting, Topological, and Magnetic Properties.

An interesting question is whether chalcogen atoms can emulate the role of carbon or boron elements stabilized between two transition metal layers, as observed in MXenes or MBenes. Here, we predict a new family of two-dimensional ternary compounds M4XY2 (where M = Pd, Y, Zr, etc.; X = S, Se, Te; and Y = Cl, Br, I), named M-chalcogene. Through first-principles calculations, we reveal diverse physical properties in these compounds, including superconducting, topological, and magnetic characteristics, where the bilayer transition metals play crucial roles. Moreover, the expected helical edge states and superconducting transition temperatures in Pd4SCl2 can be finely tuned by strains. Additionally, the Ti4SCl2 is predicted to be a topological insulator and shows promise as a gas sensor candidate for certain exotic gases. Our findings expand two-dimensional material families and provide promising platforms for diverse physical phenomena with efficient tunability by external stimuli for various applications.

Design of an Oxide Monolayer with High ZT by a Strong Anharmonicity Unit.

In this paper, a new strategy to obtain a transition-metal oxide (TMO) thermoelectric monolayer is demonstrated. We show that the TMO thermoelectric monolayer can be achieved by the replacement of a transition-metal atom with a cluster, which is composed of heavy transition atoms with abundant valence electrons. Specifically, the transition-metal atom in the XO2 (X = Ti, Zr, Hf) monolayer is replaced by the [Ag6]4+ cluster and a stable structure Ag6O2 is achieved. Due to the abundant valence electrons in the [Ag6]4+ cluster unit, n-type Ag6O2 has high electrical conductivity, which leads to a satisfactory power factor. More importantly, Ag6O2 has an extremely low phonon thermal conductivity of 0.16 W·m-1·K-1, which is one of the lowest values in thermoelectric materials. An in-depth study reveals that the extremely low value originates from the strong phonon anharmonicity and weak metal bond of the [Ag6]4+ cluster unit. Due to the satisfactory power factor and ultralow phonon thermal conductivity, Ag6O2 has high ZT at 300-700 K, and the maximum ZT is 3.77, corresponding to an energy conversion efficiency of 22.24%. Our results demonstrate that replacement of the transition-metal atom by an appropriate cluster is a good way to obtain a TMO thermoelectric monolayer.

Atomic Precision Processing of Two-Dimensional Materials for Next-Generation Microelectronics.

The growth of the information era economy is driving the pursuit of advanced materials for microelectronics, spurred by exploration into "Beyond CMOS" and "More than Moore" paradigms. Atomically thin 2D materials, such as transition metal dichalcogenides (TMDCs), show great potential for next-generation microelectronics due to their properties and defect engineering capabilities. This perspective delves into atomic precision processing (APP) techniques like atomic layer deposition (ALD), epitaxy, atomic layer etching (ALE), and atomic precision advanced manufacturing (APAM) for the fabrication and modification of 2D materials, essential for future semiconductor devices. Additive APP methods like ALD and epitaxy provide precise control over composition, crystallinity, and thickness at the atomic scale, facilitating high-performance device integration. Subtractive APP techniques, such as ALE, focus on atomic-scale etching control for 2D material functionality and manufacturing. In APAM, modification techniques aim at atomic-scale defect control, offering tailored device functions and improved performance. Achieving optimal performance and energy efficiency in 2D material-based microelectronics requires a comprehensive approach encompassing fundamental understanding, process modeling, and high-throughput metrology. The outlook for APP in 2D materials is promising, with ongoing developments poised to impact manufacturing and fundamental materials science. Integration with advanced metrology and codesign frameworks will accelerate the realization of next-generation microelectronics enabled by 2D materials.

Realization of Material with an Atomic Ruby Lattice.

The ruby lattice is one of the tight-binding models which hosts a flat band in its electronic structure and has potential applications in future spintronics and quantum devices. However, the experimental realization of a ruby lattice in realistic materials remains elusive. Here, we have experimentally realized an atomic ruby lattice by fabricating monolayer CuCl1+x on a Au(111) substrate. Scanning tunneling microscopy/spectra (STM/STS) measurements combined with density-functional theory (DFT) calculations reveal that the Cu atoms are arranged in a ruby lattice in this monolayer. Moreover, a significant density of states (DOS) peak corresponding to the characteristic of a ruby system is observed, consistent with both the tight-binding model and first-principles calculations on the band structure. Our work provides a promising platform to explore the physics of the ruby model.

Slip Opacity and Fast Osmotic Transport of Hydrophobes at Aqueous Interfaces with Two-Dimensional Materials.

We investigate the interfacial transport of water and hydrophobic solutes on van der Waals bilayers and heterostructures formed by stacking graphene, hBN, and MoS2 using extensive ab initio molecular dynamics simulations. We compute water slippage and the diffusio-osmotic transport coefficient of hydrophobic particles at the interface by combining hydrodynamics and the theory of the hydrophobic effect. We find that slippage is dominated by the layer that is in direct contact with water and only marginally altered by the second layer, leading to a so-called "slip opacity". The screening of the lateral forces, where the liquid does not feel the forces coming from the second nearest layer, is one of the factors leading to the "slip opacity" in our systems. The diffusio-osmotic transport of small hydrophobes (with a radius below 2.5 Å) is also affected by the slip opacity, being dramatically enhanced by slippage. Furthermore, the direction of diffusio-osmotic flow is controlled by the solute size, with the flow in the opposite direction of the concentration gradient for smaller hydrophobes, and vice versa for larger ones. We connect our findings to the wetting properties of two-dimensional materials, and we propose that slippage and wetting can be controlled separately: whereas the slippage is mostly determined by the layer in closer proximity to water, wetting can be finely tuned by stacking different two-dimensional materials. Our study advances the computational design of two-dimensional materials and van der Waals heterostructures, enabling precise control over wetting and slippage properties for applications in coatings and water purification membranes.

Nonvolatile Electric Control of Rashba Spin Splitting in Sb/In2Se3 Heterostructure.

Ferroelectric Rashba semiconductors (FRS) are highly demanded for their potential capability for nonvolatile electric control of electron spins. An ideal FRS is characterized by a combination of room temperature ferroelectricity and a strong Rashba effect, which has, however, been rarely reported. Herein, we designed a room-temperature FRS by vertically stacking a Sb monolayer on a room-temperature ferroelectric In2Se3 monolayer. Our first-principles calculations reveal that the Sb/In2Se3 heterostructure exhibits a clean Rashba splitting band near the Fermi level and a strong Rashba effect coupled to the ferroelectric order. Switching the electric polarization direction enhances the Rashba effect, and the flipping is feasible with a low energy barrier of 22 meV. This Rashba-ferroelectricity coupling effect is robust against changes of the heterostructure interfacial distance and external electric fields. Such a nonvolatile electrically tunable Rashba effect at room temperature enables potential applications in next-generation data storage and logic devices operated under small electrical currents.

Ternary Content-Addressable Memory Based on a Single Two-Dimensional Transistor for Memory-Augmented Learning.

Ternary content-addressable memory (TCAM) is promising for data-intensive artificial intelligence applications due to its large-scale parallel in-memory computing capabilities. However, it is still challenging to build a reliable TCAM cell from a single circuit component. Here, we demonstrate a single transistor TCAM based on a floating-gate two-dimensional (2D) ambipolar MoTe2 field-effect transistor with graphene contacts. Our bottom graphene contacts scheme enables gate modulation of the contact Schottky barrier heights, facilitating carrier injection for both electrons and holes. The 2D nature of our channel and contact materials provides device scaling potentials beyond silicon. By integration with a floating-gate stack, a highly reliable nonvolatile memory is achieved. Our TCAM cell exhibits a resistance ratio larger than 1000 and symmetrical complementary states, allowing the implementation of large-scale TCAM arrays. Finally, we show through circuit simulations that in-memory Hamming distance computation is readily achievable based on our TCAM with array sizes up to 128 cells.

Ferroelectrovalley in Two-Dimensional Multiferroic Lattices.

Engineering the valley index is essential and highly sought for valley physics, but currently, it is exclusively based on the paradigm of the challenging ferrovalley with spin-orientation reversal under a magnetic field. Here, an alternative strategy, i.e., the so-called ferroelectrovalley, is proposed to tackle the insurmountable spin-orientation reversal, which reverses the valley index with the feasible ferroelectricity. Using symmetry arguments and the tight-binding model, the C2z rotation is unveiled to be able to take the place of time reversal for operating the valley index in two-dimensional multiferroic kagome lattices, which enables a ferroelectricity-engineered valley index, thereby generating the concept of a ferroelectrovalley. Based on first-principles calculations, this concept is further demonstrated in the breathing kagome lattice of single-layer Ti3Br8, wherein ferroelectricity couples with the breathing process. These findings open a new direction for valleytronics and 2D materials research.

Monoclinic LaSb2 Superconducting Thin Films.

Rare-earth diantimondes exhibit coupling between structural and electronic orders, which are tunable under pressure and temperature. Here we present the discovery of a new polymorph of LaSb2 stabilized in thin films synthesized using molecular beam epitaxy. Using diffraction, electron microscopy, and first-principles calculations we identify a YbSb2-type monoclinic lattice as a yet-uncharacterized stacking configuration. The material hosts superconductivity with a Tc = 2 K, which is enhanced relative to the bulk ambient phase, and a long superconducting coherence length of 1730 Å. This result highlights the potential thin film growth has in stabilizing novel stacking configurations in quasi-two-dimensional compounds with competing layered structures.

Synthesis and Polymorph Manipulation of FeSe2 Monolayers.

Polymorph engineering involves the manipulation of material properties through controlled structural modification and is a candidate technique for creating unique two-dimensional transition metal dichalcogenide (TMDC) nanodevices. Despite its promise, polymorph engineering of magnetic TMDC monolayers has not yet been demonstrated. Here we grow FeSe2 monolayers via molecular beam epitaxy and find that they have great promise for magnetic polymorph engineering. Using scanning tunneling microscopy (STM) and spectroscopy (STS), we find that FeSe2 monolayers predominantly display a 1T' structural polymorph at 5 K. Application of voltage pulses from an STM tip causes a local, reversible transition from the 1T' phase to the 1T phase. Density functional theory calculations suggest that this single-layer structural phase transition is accompanied by a magnetic transition from an antiferromagnetic to a ferromagnetic configuration. These results open new possibilities for creating functional magnetic devices with TMDC monolayers via polymorph engineering.

Hummers' method-assisted liquid-phase exfoliation enables the fabrication of few-layer borophene from bulk boron.

The fabrication of few-layer borophene (BP) from bulk boron (b-B) is of great importance and still a scientific challenge due to the complex structure and crystallinity of b-B. Herein, we propose a novel technique to prepare a few-layer BP on a large scale with a large lateral size in a well-controlled manner. For this, we employed the Hummers' method-assisted liquid-phase exfoliation. In the first step, the chemical exfoliation of the b-B as a precursor was performed by the modified Hummers' method. After chemical exfoliation, mechanical delamination was employed by using an immersion sonicator. Finally, BP sheets were collected with dimensions ranging from several hundred nanometers to a few micrometers and an average thickness of 4.2 nm. We envision that the proposed low-cost, flexible, and large-scale production method will provide unique advantages for the application of few-layer BP in the realization of high-performance electronics, optoelectronics, flexible devices, sensing systems, energy conversion, and storage devices.

Antimony-Platinum Modulated Contact Enabling Majority Carrier Polarity Selection on a Monolayer Tungsten Diselenide Channel.

We develop a novel metal contact approach using an antimony (Sb)-platinum (Pt) bilayer to mitigate Fermi-level pinning in 2D transition metal dichalcogenide channels. This strategy allows for control over the transport polarity in monolayer WSe2 devices. By adjustment of the Sb interfacial layer thickness from 10 to 30 nm, the effective work function of the contact/WSe2 interface can be tuned from 4.42 eV (p-type) to 4.19 eV (n-type), enabling selectable n-/p-FET operation in enhancement mode. The shift in effective work function is linked to Sb-Se bond formation and an emerging n-doping effect. This work demonstrates high-performance n- and p-FETs with a single WSe2 channel through Sb-Pt contact modulation. After oxide encapsulation, the maximum current density at |VD| = 1 V reaches 170 µA/µm for p-FET and 165 µA/µm for n-FET. This approach shows promise for cost-effective CMOS transistor applications using a single channel material and metal contact scheme.

Emergence of Band Structure in a Two-Dimensional Metal-Organic Framework upon Hierarchical Self-Assembly.

Two-dimensional metal-organic frameworks (2D-MOFs) represent a category of atomically thin materials that combine the structural tunability of molecular systems with the crystalline structure characteristic of solids. The strong bonding between the organic linkers and transition metal centers is expected to result in delocalized electronic states. However, it remains largely unknown how the band structure in 2D-MOFs emerges through the coupling of electronic states in the building blocks. Here, we demonstrate the on-surface synthesis of a 2D-MOF exhibiting prominent π-conjugation. Through a combined experimental and theoretical approach, we provide direct evidence of band structure formation upon hierarchical self-assembly, going from metal-organic complexes to a conjugated two-dimensional framework. Additionally, we identify the robustly dispersive nature of the emerging hybrid states, irrespective of the metallic support type, highlighting the tunability of the band structure through charge transfer from the substrate. Our findings encourage the exploration of band-structure engineering in 2D-MOFs for potential applications in electronics and photonics.

High-Density Dual-Structure Single-Atom Pt Electrocatalyst for Efficient Hydrogen Evolution and Multimodal Sensing.

Herein, we report a high-density dual-structure single-atom catalyst (SAC) by creating a large number of vacancies of O and Ti in two-dimensional (2D) Ti3C2 to immobilize Pt atoms (SA Pt-Ti3C2). The SA Pt-Ti3C2 showed excellent performance toward the pH-universal electrochemical hydrogen evolution reaction (HER) and multimodal sensing. For HER catalysis, compared to the commercial 20 wt % Pt/C, the Pt mass activities of SA Pt-Ti3C2 at the overpotentials of ∼30 and 110 mV in acid and alkaline media are 45 and 34 times higher, respectively. More importantly, during the alkaline HER process, an interesting synergetic effect between Pt-C and Pt-Ti sites that dominated the Volmer and Heyrovsky steps, respectively, was revealed. Moreover, the SA Pt-Ti3C2 catalyst exhibited high sensitivity (0.62-2.65 µA µM-1) and fast response properties for the multimodal identifications of ascorbic acid, dopamine, uric acid, and nitric oxide under the assistance of machine learning.

The Impact of Microwave Annealing on MoS2 Devices Assisted by Neural Network-Based Big Data Analysis.

Microwave annealing, an emerging annealing method known for its efficiency and low thermal budget, has established a foundational research base in the annealing of molybdenum disulfide (MoS2) devices. Typically, to obtain high-quality MoS2 devices, mechanical exfoliation is commonly employed. This method's challenge lies in achieving uniform film thickness, which limits the use of extensive data for studying the effects of microwave annealing on the MoS2 devices. In this experiment, we utilized a neural network approach based on the HSV (hue, saturation, value) color space to assist in distinguishing film thickness for the fabrication of numerous MoS2 devices with enhanced uniformity and consistency. This method allowed us to precisely assess the impact of microwave annealing on device performance. We discovered a relationship between the device's electrical performance and the annealing power. By analyzing the statistical data of these electrical parameters, we identified the optimal annealing power for MoS2 devices as 700 W, providing insights and guidance for the microwave annealing process of two-dimensional materials.