Two-dimensional Electronic Materials Research Articles

Enhancing Carrier Mobility in Monolayer MoS2 Transistors with Process-Induced Strain.

Two-dimensional electronic materials are a promising candidate for beyond-silicon electronics due to their favorable size scaling of electronic performance. However, a major challenge is the heterogeneous integration of 2D materials with CMOS processes while maintaining their excellent properties. In particular, there is a knowledge gap in how thin film deposition and processes interact with 2D materials to alter their strain and doping, both of which have a drastic impact on device properties. In this study, we demonstrate how to utilize process-induced strain, a common technique extensively applied in the semiconductor industry, to enhance the carrier mobility in 2D material transistors. We systematically varied the tensile strain in monolayer MoS2 transistors by iteratively depositing thin layers of high-stress MgOx stressor. At each thickness, we combined Raman spectroscopy and transport measurements to unravel and correlate the changes in strain and doping within each transistor with their performance. The transistors displayed uniform strain distributions across their channels for tensile strains of up to 0.48 ± 0.05%, at 150 nm of stressor thickness. At higher thicknesses, mechanical instability occurred, leading to nonuniform strains. The transport characteristics systematically varied with strain, with enhancement in electron mobility at a rate of 130 ± 40% per % strain and enhancement of the channel saturation current density of 52 ± 20%. This work showcases how established CMOS technologies can be leveraged to tailor the transport in 2D transistors, accelerating the integration of 2D electronics into a future computing infrastructure.

Evidence of the fractional quantum spin Hall effect in moiré MoTe2.

Quantum spin Hall (QSH) insulators are two-dimensional electronic materials that have a bulk band gap similar to an ordinary insulator but have topologically protected pairs of edge modes of opposite chiralities1-6. So far, experimental studies have found only integer QSH insulators with counter-propagating up-spins and down-spins at each edge leading to a quantized conductance G0 = e2/h (with e and h denoting the electron charge and Planck's constant, respectively)7-14. Here we report transport evidence of a fractional QSH insulator in 2.1° twisted bilayer MoTe2, which supports spin-Sz conservation and flat spin-contrasting Chern bands15,16. At filling factor ν = 3 of the moiré valence bands, each edge contributes a conductance with zero anomalous Hall conductivity. The state is probably a time-reversal pair of the even-denominator 3/2-fractional Chern insulators. Furthermore, at ν = 2, 4 and 6, we observe a single, double and triple QSH insulator with each edge contributing a conductance G0, 2G0 and 3G0, respectively. Our results open up the possibility of realizing time-reversal symmetric non-abelian anyons and other unexpected topological phases in highly tunable moiré materials17-19.

Cavity Quantum Electrodynamics with Hyperbolic van der Waals Materials.

The ground-state properties and excitation energies of a quantum emitter can be modified in the ultrastrong coupling regime of cavity quantum electrodynamics (QED) where the light-matter interaction strength becomes comparable to the cavity resonance frequency. Recent studies have started to explore the possibility of controlling an electronic material by embedding it in a cavity that confines electromagnetic fields in deep subwavelength scales. Currently, there is a strong interest in realizing ultrastrong-coupling cavity QED in the terahertz (THz) part of the spectrum, since most of the elementary excitations of quantum materials are in this frequency range. We propose and discuss a promising platform to achieve this goal based on a two-dimensional electronic material encapsulated by a planar cavity consisting of ultrathin polar van der Waals crystals. As a concrete setup, we show that nanometer-thick hexagonal boron nitride layers should allow one to reach the ultrastrong coupling regime for single-electron cyclotron resonance in a bilayer graphene. The proposed cavity platform can be realized by a wide variety of thin dielectric materials with hyperbolic dispersions. Consequently, van der Waals heterostructures hold the promise of becoming a versatile playground for exploring the ultrastrong-coupling physics of cavity QED materials.

Area-Specific, Hierarchical Nanowrinkling of Two-Dimensional Materials.

This paper describes an approach to generate hierarchical wrinkles in two-dimensional (2D) electronic materials with spatial control over adjacent wavelengths. A rigid fluoropolymer mold was used to pattern a sacrificial polymer skin layer on monolayer graphene, molybdenum disulfide, and hexagonal boron nitride on prestrained thermoplastic sheets. Strain relief and removal of the polymer layer resulted in 2D-material wrinkles whose wavelengths scaled linearly with the local skin thickness. A second generation of wrinkles could be created on top of the first generation by applying a subsequent cycle of polymer skin coating, strain relief, and polymer removal. This area-specific hierarchical wrinkling is general and will facilitate the engineering of the local properties of various 2D materials and their heterostructures.

Band structures of graphene, black phosphorus, and MoS2 ribbons under stress: a comparison study

The application of electronic devices becomes increasingly extensive and their performance optimization receives broad attention. Electronic devices constructed from two-dimensional materials have revealed broad prospects. However, the performance of two-dimensional electronic materials in the presence of stress has rarely been researched, which will restrict their application in an environment with intense deformation or temperature variation. Here, we adopt a first-principle method to investigate three kinds of ribbons: graphene, black phosphorus, and MoS2. We find that the bandgap of graphene and MoS2 ribbons increase with the rise of stress, while the bandgap of black phosphorus reduces when subject to both positive and negative stress. The abnormal trend of black phosphorus is owing to the indirect bandgap properties under negative stress, which becomes direct bandgap under positive stress. The present research has instructive meaning for the application of two-dimensional material on electronic devices under stressed conditions.

Chemically Exfoliated Titanium Carbide MXene for Highly Sensitive Electrochemical Sensors for Detection of 4-Nitrophenols in Drinking Water.

Soil and water contamination by numerous pollutants has been increasingly posing threats to food, water, agriculture, and human health. Using novel nanoscale materials to develop rapid electrochemical sensors is very promising due to the discovery of a number of new two-dimensional (2D) electronic materials. Of particular importance is 2D transition-metal carbide MXene that has been shown to possess transformative properties pertaining to its physical, chemical, and environmental characteristics, leading to their potential sensor applications. Designing electrochemical sensors using MXene has the potential to pave the way for monitoring environmental pollutants. Here, a stacked layer of chemically exfoliated MXene (Ti3C2T x ) was demonstrated as an electrochemical sensor for detection of 4-nitrophenol (4-NP) with high sensitivity and a low limit of detection. Successful selective exfoliation of the MAX (Ti3AlC2) phase of the material by chemical etching without oxidation is shown to be the key to achieving higher sensitivity and a lower detection limit. In the optimal conditions, the proposed MXene sensor electrodes were capable of detecting 4-NP in a broad concentration range from 500 nM to 100 μM with a good linear sensing range (regression fit, R = 0.995). The higher sensitivity and notable limit of detection reached about 16.35 μA μM-1 cm-2 and 42 nM/L, respectively, with good reproducibility and repeatability. The real-time application of the proposed MXene sensor electrodes was confirmed by testing in tap water samples with excellent recoveries of 95-99%.

Functionalized graphene-based nanocomposites for smart optoelectronic applications

Abstract The recent increase in the use of graphene and its derivatives is due to their exceptional physicochemical, electrical, mechanical, and thermal properties as the industrial materials developed by involving graphene structures can fulfill future needs. In that view, the potential use of these graphene-containing nanomaterials in electronics applications has encouraged in-depth exploration of the electronic, conducting, and other functional properties. The protecting undifferentiated form of graphene has similarly been proposed for various applications, for example, as supercapacitors, photovoltaic and transparent conductors, touch screen points, optical limiters, optical frequency converters, and terahertz devices. The hybrid composite nanomaterials that undergo stimulus-induced optical and electrical changes are important for many new technologies based on switchable devices. As a two-dimensional smart electronic material, graphene has received widespread attention, and with that view, we aim to cover the various types of graphene oxide (GO)-based composites, linking their optical and electrical properties with their structural and morphological ones. We believe that the topics covered in this review can shed light on the development of high-yield GO-containing electronic materials, which can be fabricated as the field moves forward and makes more significant advances in smart optoelectronic devices.

Strain-induced work function in h-BN and BCN monolayers

Abstract In the last decade, research activities of semiconducting two-dimensional (2D) electronic materials has received widespread attention, and the work function analysis is a significant parameter for investigating the feasible optoelectronic activity of these 2D materials. Here, we report a comparative study using ab-inito based density functional theory calculations to examine the impact of uniaxial and biaxial tensile and compressive strains on the work functions of boron nitride (h-BN) and boron carbonitride (BCN) monolayers. Unlike h-BN which has a large bandgap of 5 eV, the computed direct bandgap of BCN monolayer is 1.18 eV, which is beneficial for use in optoelectronic applications. We noticed that the calculated work function of both h-BN and BCN decreases (increases) continuously by increasing the compressive (tensile) strain irrespective of the strain directions. The observed variations in the work function in both h-BN and BCN are found to be related to the modulation of Fermi energy under compressive and tensile strains. The change in bond length between the atoms changes the total energy as a function of applied strain. Moreover, the direct bandgaps of both h-BN and BCN remain unaffected within the studied range of compressive and tensile strains, which can be beneficial for their use in photovoltaic devices. We also noticed that elastic modulus and Poisson's ratio are found to be anisotropic and decrease (increase) with the application of uniaxial tensile (compressive) strain. In addition, both h-BN and BCN possess high longitudinal and transverse wave velocities. The insight gained from this study will stimulate the research on BCN in view of relevant technological applications in the fields of nanoelectronics and optoelectronics.

Direct laser writing of graphene electrodes

Direct laser writing of graphene electrodes is an emerging research field for the rapid fabrication of two-dimensional carbon electronic materials with wide applications, ranging from supercapacitors and batteries to sensors, electrocatalysts, actuators, etc. Many types of carbon-containing raw materials can be converted to graphene by one-step laser scribing, without complicated chemical synthesis routines, using a variety of lasers. This perspective categorizes the principles of direct laser writing of graphene, according to the different types of raw materials, different types of lasers, and different applications. The future directions of laser synthesized graphene are also discussed.

Two-dimensional spin-valley locking spin valve

Valleytronics is an emerging field of research which employs energy valleys in the band structure of two-dimensional (2D) electronic materials to encode information. A special interest has been triggered by the associated spin-valley coupling which reveals rich fundamental physics and enables new functionalities. Here, we propose exploiting the spin-valley locking in 2D materials with a large spin-orbit coupling and electric-field reversible valley spin polarization, such as germanene, stanene, a $1{T}^{\ensuremath{'}}$ transition metal dichalcogenide (TMDC) monolayer, and a $2H$-TMDC bilayer, to realize a valley spin valve (VSV). The valley spin polarization in these materials can be switched by an external electric field, which enables functionalities of a valley spin polarizer or a valley spin analyzer. When placed in series, they constitute the proposed VSV---a device whose conductance state is ON or OFF depending on the relative valley spin polarization of the polarizer and the analyzer. Using quantum-transport calculations based on an adequate tight-binding model, we predict a giant VSV ratio of nearly 100% for both germanene- and stanene-based VSV devices. Our results demonstrate the implication of the spin-valley coupling in 2D materials for the novel device concept promising for valleytronics.

Platform for Electrically Pumped Polariton Simulators and Topological Lasers.

Two-dimensional electronic materials such as graphene and transition metal dichalgenides feature unique electrical and optical properties due to the conspirative effect of band structure, orbital coupling, and crystal symmetry. Synthetic matter, as accomplished by artificial lattice arrangements of cold atoms, molecules, electron patterning, and optical cavities, has emerged to provide manifold intriguing frameworks to likewise realize such scenarios. Exciton polaritons have recently been added to the list of promising candidates for the emulation of system Hamiltonians on a semiconductor platform, offering versatile tools to engineer the potential landscape and to access the nonlinear electro-optical regime. In this work, we introduce an electronically driven square and honeycomb lattice of exciton polaritons, paving the way towards real world devices based on polariton lattices for on-chip applications. Our platform exhibits laserlike emission from high-symmetry points under direct current injection, hinting at the prospect of electrically driven polariton lasers with possibly topologically nontrivial properties.

Method irons out 2-D materials for computer chips

Two-dimensional electronic materials could be key ingredients in future energy-efficient computer chips—if engineers can learn to build devices with them. On Dec. 4 at the International Electron Devices Meeting in San Francisco, researchers from the Belgian semiconductor research company Imec presented a method for making and transferring smooth, high-quality sheets of tungsten disulfide and other 2-D materials. Devices with 2-D materials have been made in the lab but they tend to be one-offs. “We’re always limited by the precision of lab tools,” says Imec device physicist Iuliana Radu. Her team sought a way to transfer large sheets of 2-D materials from the surface on which they are grown, to the surface of a silicon wafer patterned with electronic circuits, without wrinkling the 2-D material or melting the underlying silicon devices. They grew a WS2 film, 0.7 nm thick and 300 mm in diameter, on a silicon wafer. They attached the

Colloidal nanoelectronic state machines based on 2D materials for aerosolizable electronics

A previously unexplored property of two-dimensional electronic materials is their ability to graft electronic functionality onto colloidal particles to access local hydrodynamics in fluids to impart mobility and enter spaces inaccessible to larger electronic systems. Here, we demonstrate the design and fabrication of fully autonomous state machines built onto SU-8 particles powered by a two-dimensional material-based photodiode. The on-board circuit connects a chemiresistor circuit element and a memristor element, enabling the detection and storage of information after aerosolization, hydrodynamic propulsion to targets over 0.6 m away, and large-area surface sensing of triethylamine, ammonia and aerosolized soot in inaccessible locations. An incorporated retroreflector design allows for facile position location using laser-scanning optical detection. Such state machines may find widespread application as probes in confined environments, such as the human digestive tract, oil and gas conduits, chemical and biosynthetic reactors, and autonomous environmental sensors.

Largely Tunable Band Structures of Few-Layer InSe by Uniaxial Strain.

Because of the strong quantum confinement effect, few-layer γ-InSe exhibits a layer-dependent band gap, spanning the visible and near infrared regions, and thus recently has been drawing tremendous attention. As a two-dimensional material, the mechanical flexibility provides an additional tuning knob for the electronic structures. Here, for the first time, we engineer the band structures of few-layer and bulk-like InSe by uniaxial tensile strain and observe a salient shift of photoluminescence peaks. The shift rate of the optical gap is approximately 90-100 meV per 1% strain for four- to eight-layer samples, which is much larger than that for the widely studied MoS2 monolayer. Density functional theory calculations well reproduce the observed layer-dependent band gaps and the strain effect and reveal that the shift rate decreases with the increasing layer number for few-layer InSe. Our study demonstrates that InSe is a very versatile two-dimensional electronic and optoelectronic material, which is suitable for tunable light emitters, photodetectors, and other optoelectronic devices.

Model for the Operation of a Monolayer MoS2 Thin-Film Transistor with Charges Trapped near the Channel Interface

Two-dimensional electronic materials are a dream come true for creating thin-film transistors (TFTs), and here monolayer transition-metal dichalcogenides can be even more appealing than graphene, as they present a natural band gap. An understanding of the physics behind observed device behavior is still needed, though. The authors calculate the $I-V$ characteristics of a system with high charge density near the channel interface, then build an actual MoS${}_{2}$ TFT to compare. Strong agreement with experiment shows that their model can quantify the densities of trap sites and trapped charge based on simple measurements of transfer curves.

Band Alignment in the Single-Layer MoS2/WSe2 Heterojunction

The emergence of transition metal dichalcogenides as two-dimensional electronic materials has stimulated proposals of novel electronic and photonic devices based on the heterostructures of transition metal dichalcogenides (TMDs). The band alignment for TMD heterostructures is practically important for applications. We examined the feasibility of Electron Affinity Rule (EAR) on TMD heterojunction band alignment by stand-alone X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS). Our results suggest that the EAR can successfully predict the band alignment of TMD heterostructures.

Determination of band alignment in the single-layer MoS2/WSe2 heterojunction.

The emergence of two-dimensional electronic materials has stimulated proposals of novel electronic and photonic devices based on the heterostructures of transition metal dichalcogenides. Here we report the determination of band offsets in the heterostructures of transition metal dichalcogenides by using microbeam X-ray photoelectron spectroscopy and scanning tunnelling microscopy/spectroscopy. We determine a type-II alignment between MoS2 and WSe2 with a valence band offset value of 0.83 eV and a conduction band offset of 0.76 eV. First-principles calculations show that in this heterostructure with dissimilar chalcogen atoms, the electronic structures of WSe2 and MoS2 are well retained in their respective layers due to a weak interlayer coupling. Moreover, a valence band offset of 0.94 eV is obtained from density functional theory, consistent with the experimental determination.

Tuning the band gap in silicene by oxidation.

Silicene monolayers grown on Ag(111) surfaces demonstrate a band gap that is tunable by oxygen adatoms from semimetallic to semiconducting type. With the use of low-temperature scanning tunneling microscopy, we find that the adsorption configurations and amounts of oxygen adatoms on the silicene surface are critical for band gap engineering, which is dominated by different buckled structures in √13 × √13, 4 × 4, and 2√3 × 2√3 silicene layers. The Si-O-Si bonds are the most energy-favored species formed on √13 × √13, 4 × 4, and 2√3 × 2√3 structures under oxidation, which is verified by in situ Raman spectroscopy as well as first-principles calculations. The silicene monolayers retain their structures when fully covered by oxygen adatoms. Our work demonstrates the feasibility of tuning the band gap of silicene with oxygen adatoms, which, in turn, expands the base of available two-dimensional electronic materials for devices with properties that is hardly achieved with graphene oxide.

Metallized DNA nanolithography for encoding and transferring spatial information for graphene patterning

The vision for graphene and other two-dimensional electronics is the direct production of nanoelectronic circuits and barrier materials from a single precursor sheet. DNA origami and single-stranded tiles are powerful methods to encode complex shapes within a DNA sequence, but their translation to patterning other nanomaterials has been limited. Here we develop a metallized DNA nanolithography that allows transfer of spatial information to pattern two-dimensional nanomaterials capable of plasma etching. Width, orientation and curvature can be programmed by specific sequence design and transferred, as we demonstrate for graphene. Spatial resolution is limited by distortion of the DNA template upon Au metallization and subsequent etching. The metallized DNA mask allows for plasmonic enhanced Raman spectroscopy of the underlying graphene, providing information on defects, doping and lattice symmetry. This DNA nanolithography enables wafer-scale patterning of two-dimensional electronic materials to create diverse circuit elements, including nanorings, three- and four-membered nanojunctions, and extended nanoribbons.

Beyond Graphene: Silicene and Germanene Novel Two-Dimensional Electronic Materials

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