Can 2D Semiconductors Be Game-Changers for Nanoelectronics and Photonics?

2D semiconductors have interesting physical and chemical attributes that have led them to become one of the most intensely investigated semiconductor families in recent history. They may play a crucial role in the next technological revolution in electronics as well as optoelectronics or photonics. In this Perspective, we explore the fundamental principles and significant advancements in electronic and photonic devices comprising 2D semiconductors. We focus on strategies aimed at enhancing the performance of conventional devices and exploiting important properties of 2D semiconductors that allow fundamentally interesting device functionalities for future applications. Approaches for the realization of emerging logic transistors and memory devices as well as photovoltaics, photodetectors, electro-optical modulators, and nonlinear optics based on 2D semiconductors are discussed. We also provide a forward-looking perspective on critical remaining challenges and opportunities for basic science and technology level applications of 2D semiconductors.

Tuning Polarity in WSe2/AlScN FeFETs via Contact Engineering.

Recent advancements in ferroelectric field-effect transistors (FeFETs) using two-dimensional (2D) semiconductor channels and ferroelectric Al0.68Sc0.32N (AlScN) allow high-performance nonvolatile devices with exceptional ON-state currents, large ON/OFF current ratios, and large memory windows (MW). However, previous studies have solely focused on n-type FeFETs, leaving a crucial gap in the development of p-type and ambipolar FeFETs, which are essential for expanding their applicability to a wide range of circuit-level applications. Here, we present a comprehensive demonstration of n-type, p-type, and ambipolar FeFETs on an array scale using AlScN and multilayer/monolayer WSe2. The dominant injected carrier type is modulated through contact engineering at the metal-semiconductor junction, resulting in the realization of all three types of FeFETs. The effect of contact engineering on the carrier injection is further investigated through technology-computer-aided design simulations. Moreover, our 2D WSe2/AlScN FeFETs achieve high electron and hole current densities of ∼20 and ∼10 µA/µm, respectively, with a high ON/OFF ratio surpassing ∼107 and a large MW of >6 V (0.14 V/nm).

Tunable Localized Charge Transfer Excitons in Nanoplatelet-2D Chalcogenide van der Waals Heterostructures.

Observation of interlayer, charge transfer (CT) excitons in van der Waals heterostructures (vdWHs) based on 2D-2D systems has been well investigated. While conceptually interesting, these charge transfer excitons are highly delocalized and spatially localizing them requires twisting layers at very specific angles. This issue of localizing the CT excitons can be overcome via making nanoplate-2D material heterostructures (N2DHs) where one of the components is a spatially quantum confined medium. Here, we demonstrate the formation of CT excitons in a mixed dimensional system comprising MoSe2 and WSe2 monolayers and CdSe/CdS-based core/shell nanoplates (NPLs). Spectral signatures of CT excitons in our N2DHs were resolved locally at the 2D/single-NPL heterointerface using tip-enhanced photoluminescence (TEPL) at room temperature. By varying both the 2D material and the shell thickness of the NPLs and applying an out-of-plane electric field, the exciton resonance energy was tuned by up to 100 meV. Our finding is a significant step toward the realization of highly tunable N2DH-based next-generation photonic devices.

Vertical van der Waals heterojunction diodes comprising 2D semiconductors on 3D ß-Ga2O3.

Wide bandgap semiconductors such as gallium oxide (Ga2O3) have attracted much attention for their use in next-generation high-power electronics. Although single-crystal Ga2O3 substrates can be routinely grown from melt along various orientations, the influence of such orientations has been seldom reported. Further, making rectifying p-n diodes from Ga2O3 has been difficult due to lack of p-type doping. In this study, we fabricated and optimized 2D/3D vertical diodes on ß-Ga2O3 by varying the following three factors: substrate planar orientation, choice of 2D material and metal contacts. The quality of our devices was validated using high-temperature dependent measurements, atomic-force microscopy (AFM) techniques and technology computer-aided design (TCAD) simulations. Our findings suggest that 2D/3D ß-Ga2O3 vertical heterojunctions are optimized by substrate planar orientation (-201), combined with 2D WS2 exfoliated layers and Ti contacts, and show record rectification ratios (>106) concurrently with ON-Current density (>103 A cm-2) for application in power rectifiers.

Fabrication of p-type 2D single-crystalline transistor arrays with Fermi-level-tuned van der Waals semimetal electrodes.

High-performance p-type two-dimensional (2D) transistors are fundamental for 2D nanoelectronics. However, the lack of a reliable method for creating high-quality, large-scale p-type 2D semiconductors and a suitable metallization process represents important challenges that need to be addressed for future developments of the field. Here, we report the fabrication of scalable p-type 2D single-crystalline 2H-MoTe2 transistor arrays with Fermi-level-tuned 1T'-phase semimetal contact electrodes. By transforming polycrystalline 1T'-MoTe2 to 2H polymorph via abnormal grain growth, we fabricated 4-inch 2H-MoTe2 wafers with ultra-large single-crystalline domains and spatially-controlled single-crystalline arrays at a low temperature (~500 °C). Furthermore, we demonstrate on-chip transistors by lithographic patterning and layer-by-layer integration of 1T' semimetals and 2H semiconductors. Work function modulation of 1T'-MoTe2 electrodes was achieved by depositing 3D metal (Au) pads, resulting in minimal contact resistance (~0.7 kΩ·µm) and near-zero Schottky barrier height (~14 meV) of the junction interface, and leading to high on-state current (~7.8 µA/µm) and on/off current ratio (~105) in the 2H-MoTe2 transistors.

Scalable CMOS back-end-of-line-compatible AlScN/two-dimensional channel ferroelectric field-effect transistors.

Three-dimensional monolithic integration of memory devices with logic transistors is a frontier challenge in computer hardware. This integration is essential for augmenting computational power concurrent with enhanced energy efficiency in big data applications such as artificial intelligence. Despite decades of efforts, there remains an urgent need for reliable, compact, fast, energy-efficient and scalable memory devices. Ferroelectric field-effect transistors (FE-FETs) are a promising candidate, but requisite scalability and performance in a back-end-of-line process have proven challenging. Here we present back-end-of-line-compatible FE-FETs using two-dimensional MoS2 channels and AlScN ferroelectric materials, all grown via wafer-scalable processes. A large array of FE-FETs with memory windows larger than 7.8 V, ON/OFF ratios greater than 107 and ON-current density greater than 250 µA um-1, all at ~80 nm channel length are demonstrated. The FE-FETs show stable retention up to 10 years by extension, and endurance greater than 104 cycles in addition to 4-bit pulse-programmable memory features, thereby opening a path towards the three-dimensional heterointegration of a two-dimensional semiconductor memory with silicon complementary metal-oxide-semiconductor logic.

Air-stable van der Waals PtTe2 conductors with high current-carrying capacity and strong spin-orbit interaction.

High-performance van der Waals (vdW) integrated electronics and spintronics require reliable current-carrying capacity. However, it is challenging to achieve high current density and air-stable performance using vdW metals owing to the fast electrical breakdown triggered by defects or oxidation. Here, we report that spin-orbit interacted synthetic PtTe2 layers exhibit significant electrical reliability and robustness in ambient air. The 4-nm-thick PtTe2 synthesized at a low temperature (∼400°C) shows intrinsic metallic transport behavior and a weak antilocalization effect attributed to the strong spin-orbit scattering. Remarkably, PtTe2 sustains a high current density approaching ≈31.5 MA cm-2, which is the highest value among electrical interconnect candidates under oxygen exposure. Electrical failure is caused by the Joule heating of PtTe2 rather than defect-induced electromigration, which was achievable by the native TeOx passivation. The high-quality growth of PtTe2 and the investigation of its transport behaviors lay out essential foundations for the development of emerging vdW spin-orbitronics.

Atomic transistors based on seamless lateral metal-semiconductor junctions with a sub-1-nm transfer length.

The edge-to-edge connected metal-semiconductor junction (MSJ) for two-dimensional (2D) transistors has the potential to reduce the contact length while improving the performance of the devices. However, typical 2D materials are thermally and chemically unstable, which impedes the reproducible achievement of high-quality edge contacts. Here we present a scalable synthetic strategy to fabricate low-resistance edge contacts to atomic transistors using a thermally stable 2D metal, PtTe2. The use of PtTe2 as an epitaxial template enables the lateral growth of monolayer MoS2 to achieve a PtTe2-MoS2 MSJ with the thinnest possible, seamless atomic interface. The synthesized lateral heterojunction enables the reduced dimensions of Schottky barriers and enhanced carrier injection compared to counterparts composed of a vertical 3D metal contact. Furthermore, facile position-selected growth of PtTe2-MoS2 MSJ arrays using conventional lithography can facilitate the design of device layouts with high processability, while providing low contact resistivity and ultrashort transfer length on wafer scales.

Synthesis of high quality 2D carbide MXene flakes using a highly purified MAX precursor for ink applications.

The practical application of 2D MXenes in electronic and energy fields has been hindered by the severe variation in the quality of MXene products depending on the parent MAX phases, manufacturing techniques, and preparation parameters. In particular, their synthesis has been impeded by the lack of studies reporting the synthesis of high-quality parent MAX phases. In addition, controllable and uniform deposition of 2D MXenes on various large-scale substrates is urgently required to use them practically. Herein, a method of pelletizing raw materials could synthesize a stoichiometric Ti3AlC2 MAX phase with high yield and processability, and fewer impurities. The Ti3AlC2 could be exfoliated into 1-2-atom-thick 2D Ti3C2T x flakes, and their applicability was confirmed by the deposition and additional alignment of the 2D flakes with tunable thickness and electrical properties. Moreover, a practical MXene ink was fabricated with rheological characterization. MXene ink exhibited much better thickness uniformity while retaining excellent electrical performances (e.g., sheet resistance, electromagnetic interference shielding ability) as those of a film produced by vacuum filtration. The direct functional integration of MXenes on various substrates is expected to initiate new and unexpected MXene-based applications.

Antiphase Boundaries as Faceted Metallic Wires in 2D Transition Metal Dichalcogenides.

Antiphase boundaries (APBs) in 2D transition metal dichalcogenides have attracted wide interest as 1D metallic wires embedded in a semiconducting matrix, which could be exploited in fully 2D-integrated circuits. Here, the anisotropic morphologies of APBs (i.e., linear and saw-toothed APBs) in the nanoscale are investigated. The experimental and computational results show that despite their anisotropic nanoscale morphologies, all APBs adopt a predominantly chalcogen-oriented dense structure to maintain the energetically most stable atomic configuration. Moreover, the effect of the nanoscale morphology of an APB on electron transport from two-probe field effect transistor measurements is investigated. A saw-toothed APB has a considerably lower electron mobility than a linear APB, indicating that kinks between facets are the main factors of scattering. The observations contribute to the systematical understanding of the faceted APBs and its impact on electrical transport behavior and it could potentially extend the applications of 2D materials through defect engineering to achieve the desired properties.

Ultrathin Graphene Intercalation in PEDOT:PSS/Colorless Polyimide-Based Transparent Electrodes for Enhancement of Optoelectronic Performance and Operational Stability of Organic Devices.

A novel flexible transparent electrode (TE) having a trilayer-stacked geometry and high optoelectronic performance and operational stability was fabricated by the spin coating method. The trilayer was composed of an ultrathin graphene (Gr) film sandwiched between a transparent and colorless polyimide (TCPI) layer and a methanesulfonic acid (MSA)-treated poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) layer containing dimethylsulfoxide and Zonyl fluorosurfactant (designated as MSA-PDZ film). The introduction of solution-processable TCPI enabled the direct formation of high-quality graphene on organic surfaces with a clean interface. Stable doping of graphene with the MSA-PDZ film enabled tuning of the inherent work function and optoelectronic properties of the PEDOT:PSS films, leading to a high figure of merit of ∼70 in the as-fabricated TEs. Particularly, from multivariate and repetitive harsh environmental tests ( T = -50 to 90 °C, over 90 RH%), the TCPI/Gr heterostructure exhibited excellent tolerance to mechanical and thermal stresses and gas barrier properties that protected the MSA-PDZ film from exposure to moisture. Owing to the synergetic effect from the TCPI/Gr/MSA-PDZ anode structure, the TCPI/Gr/MSA-PDZ-based polymer light-emitting diodes showed highly improved current and power efficiencies with maxima as high as 20.84 cd/A and 22.92 lm/W, respectively (comparable to those of indium tin oxide based PLEDs), in addition to much enhanced mechanical flexibility.

Electrically Robust Single-Crystalline WTe2 Nanobelts for Nanoscale Electrical Interconnects.

As the elements of integrated circuits are downsized to the nanoscale, the current Cu-based interconnects are facing limitations due to increased resistivity and decreased current-carrying capacity because of scaling. Here, the bottom-up synthesis of single-crystalline WTe2 nanobelts and low- and high-field electrical characterization of nanoscale interconnect test structures in various ambient conditions are reported. Unlike exfoliated flakes obtained by the top-down approach, the bottom-up growth mode of WTe2 nanobelts allows systemic characterization of the electrical properties of WTe2 single crystals as a function of channel dimensions. Using a 1D heat transport model and a power law, it is determined that the breakdown of WTe2 devices under vacuum and with AlO x capping layer follows an ideal pattern for Joule heating, far from edge scattering. High-field electrical measurements and self-heating modeling demonstrate that the WTe2 nanobelts have a breakdown current density approaching ≈100 MA cm-2, remarkably higher than those of conventional metals and other transition-metal chalcogenides, and sustain the highest electrical power per channel length (≈16.4 W cm-1) among the interconnect candidates. The results suggest superior robustness of WTe2 against high-bias sweep and its possible applicability in future nanoelectronics.

Single-Crystalline Nanobelts Composed of Transition Metal Ditellurides.

Following the celebrated discovery of graphene, considerable attention has been directed toward the rich spectrum of properties offered by van der Waals crystals. However, studies have been largely limited to their 2D properties due to lack of 1D structures. Here, the growth of high-yield, single-crystalline 1D nanobelts composed of transition metal ditellurides at low temperatures (T ≤ 500 °C) and in short reaction times (t ≤ 10 min) via the use of tellurium-rich eutectic metal alloys is reported. The synthesized semimetallic 1D products are highly pure, stoichiometric, structurally uniform, and free of defects, resulting in high electrical performances. Furthermore, complete compositional tuning of the ternary ditelluride nanobelts is achieved with suppressed phase separation, applicable to the creation of unprecedented low-dimensional materials/devices. This approach may inspire new growth/fabrication strategies of 1D layered nanostructures, which may offer unique properties that are not available in other materials.