TMDC-based Devices Research Articles

(Invited, Digital Presentation) Low Voltage Operation of CMOS Inverter Based on WSe2 n/p FETs

Transition metal dichalcogenides (TMDC) have remarkable properties for the next generation of electronic devices [1]. A complementary metal-oxide-semiconductor (CMOS) inverter consisting of pairs of p-type and n-type field-effect transistor (FET) is a fundamental building block in modern digital electronics [2]. Therefore, realization of both p-type and n-type FETs based on semiconducting TMDC is of particular importance. Among various semiconducting TMDC, tungsten diselenide (WSe2) is a promising candidate for constructing a CMOS inverter because of its high mobility, symmetric electron and hole effective mass and ambipolar transport [3]. These prominent features of WSe2 motivates the fabrication and characterization of a CMOS inverter. One of the significant challenges is to develop a high-gain CMOS inverter for operation at a low power supply voltage (Vdd) for future low power digital electronics. Previous studies on a WSe2 CMOS inverter were limited to operation with a low gain of 3 or a high Vdd of more than 1 V under conditions of relatively low gate capacitance and degraded interfacial properties [3-5]. This study addressed these issues by developing a doping technique and gate stack technology to demonstrate the high-gain with low-Vdd operation of a WSe2 CMOS inverter [6]. The focus is on the doping technique of both electrons and holes to a WSe2 layer by simple spin-coating. Of particular interest in this study is the impact of gate stack technology on the CMOS inverter characteristics in low-Vdd operation. In this study, a hybrid self-assembled monolayer (SAM)/aluminum oxide (AlOx) gate dielectric is applied to a WSe2 CMOS inverter for high-gain low-Vdd operation since superior interfacial properties with high gate capacitance have been reported in molybdenum disulfide (MoS2) FETs.For p-type WSe2 FETs, the fluoropolymer CYTOP (AGC, CTX-809A) was applied since polarization in CYTOP due to the difference in electronegativity between C–F bonds generates holes in WSe2. On the other hand, poly(vinyl alcohol) (PVA) was utilized for n-type WSe2 FETs because positive charges in PVA accumulates electrons in WSe2. The resin solutions of both CYTOP and PVA were purchased from a commercial supplier. A heavily doped p-type silicon substrate (p+-Si) was thermally oxidized to form a 60 nm thick silicon dioxide (SiO2) layer for the global back-gate architecture. Palladium (Pd) and gold (Au) as the source and drain contacts for p-type and n-type WSe2 FETs were fabricated by the lift-off process, respectively. An aluminum (Al) gate was prepared and a hybrid SAM/AlOx gate dielectric was formed by oxygen (O2) plasma and an immersion process. After that, mechanically exfoliated WSe2 was transferred with a poly(dimethylsiloxane) (PDMS) stamp. Finally, CYTOP and PVA were deposited by spin-coating for p-type and n-type WSe2 FETs, respectively.Figures 1 (a) and (b) show the Id–Vg characteristics of fabricated FETs. For the p-type WSe2 FET, a small SS of 78 mV/dec and an on/off ratio of about 106 order were observed. On the other hand, the Id–Vg characteristics of the n-type WSe2 FET were degraded compared with those of the p-type WSe2 FET because of the Schottky contacts.Figures 2 (a) and (b) show the transfer characteristics and gain as a function of Vdd in CMOS inverter. The gain of the CMOS inverter increased to as high as 9 at Vdd of 0.5 V.Figure 3 shows the benchmark of this study. Our proposed concepts enabled the operation with high gain at a low Vdd as low as 0.5 V for the WSe2 CMOS inverter, which had not been realized in previous studies. The dangling-bond-free and ultrathin SAM/AlOx gate dielectric has an important role in the low-Vdd operation of the WSe2 CMOS inverter. This study opens up interesting directions for the research and development of TMDC-based devices and circuits.

Novel Design of 0D Nanoparticles-2D Transition-Metal Dichalcogenides Heterostructured Devices for High-Performance Optical and Gas-Sensing Applications

Two-dimensional Transition metal dichalcogenides (TMDCs), have now attracted much attention due to their unique layered structure and physical properties. Up to date, several studies have demonstrated monolayered and few-layered TMDC-based photodetectors with good stability, photo-switching time and broadband detectivity from UV to infrared light region. However, the reported responsivity is not as high as the theoretical expectation, indicating that the light absorption is limited by the atomic thickness of 2D-TMDCs and could still be improved. To overcome the drawback of low absorption in 2D TMDC materials, previous reports have revealed several strategies to enhance the electric field and light-harvesting in these atomically thin TMDC layers by hybridizing plasmonic noble-metal nanoparticles, such as Pt, Au and Ag, to facilitate the light-matter interaction at the surface of semiconductors. In this regard, we aim to combine highly absorptive CuInS2(CIS) nanocrystals with noble metal nanoparticles as the photosensitizer to enhance the intrinsic absorptivity and promote the performance of MoS2-based photodetectors. The interests of noble nanocrystals such as platinum and gold are featured for their distinctive properties of the carrier transportation and the storage when combined with semiconductor materials. The strategy described here acts as a perspective to significantly improve the performance of MoS2-based photodetectors with outstanding detection responsivity with selectable wavelengths by further controlling the size and material of the decorated CIS nanocrystals.In addition to optical sensing, TMDCs have also been developed as a promising candidate for gas-molecule detection. Different from commercial metal oxide gas sensors, TMDCs as sensing materials can be operated at room temperature with good performance, increasing its reliability for future industrial applications. Nevertheless, the relatively low response and long response/recovery time are the main drawbacks of these promising devices. Therefore, we proposed the approach to successfully increase the surface area of TMDCs by a one-step synthesis from WO3 into three-dimensional (3D) WS2 nanowalls through a rapid heating and rapid cooling process. Moreover, the combination of CdS/ZnS or CdSe/ZnS core/shell quantum dots (QDs) with different emission wavelengths and WS2 nanowalls will further improve the performance of WS2-based photodetector devices, including 3.5~4.7 times photocurrent enhancement and shorter response time. The remarkable results of the QD-WS2 hybrid devices to the high non-radiative energy transfer (NRET) efficiency between QDs and our nanostructured material are caused by the spectral overlap between the emission of QDs as the donors and the absorption of WS2 as the acceptors. Additionally, the outstanding NO2 gas-sensing properties of QDs/WS2 devices were demonstrated with a remarkably low detection limit down to 50 ppb with a fast response time of 26.8 s, contributed by tremendous local p-n junctions generated from p-type WS2 nanowalls and n-type CdSe-ZnS QDs in this hybrid system.Our strategies to combine 0D nanoparticles or quantum dots and 2D TMDC materials can significantly enhance the optical sensing and gas molecule sensing properties compared to pristine TMDC-based devices, resulting from the efficient charge or energy transfer between the multi-dimension material system and the creation of local p-n junctions. Moreover, the scalability of these hybrid nanostructures allows our devices to exhibit much more possibilities in advanced multifunctional applications.

Synthesis of MoS2 Thin Film by Ionized Jet Deposition: Role of Substrate and Working Parameters

The lack of scalable synthesis of transition metal dichalcogenides, such as molybdenum disulfide (MoS2), has proved to be a significant bottleneck in realization of fundamental devices and has hindered the commercialization of these materials in technologically relevant applications. In this study, a cost-efficient and versatile thin-film fabrication technique based on ionized jet deposition (IJD), i.e., a technique potentially providing high processing efficiency and scalability, is used to grow MoS2 thin films on silicon substrates. The operating conditions of IJD were found to influence mainly the ablation efficiency of the target and only slightly the quality of the deposited MoS2 thin film. All as-deposited films show chemical properties typical of MoS2 with an excess of free, elemental sulfur that can be removed by post-deposition annealing at 300–400 °C, which also promotes MoS2 crystallization. The formation of an interface comprised of several silicon oxide species was observed between MoS2 and the silicon substrate, which is suggested to originate from etching and oxidizing processes of dissociated water molecules in the vacuum chamber during growth. The present study paves the way to further design and improve the IJD approach for TMDC-based devices and other relevant technological applications.

Strong coupling between excitons and guided modes in WS2-based nanostructures

Transition-metal dichalcogenides (TMDCs) exhibit great potential in light–matter interaction due to their semiconducting nature and remarkable excitonic properties. Here a simple guided resonance structure is proposed to numerically investigate and realize dual-band light absorption exploiting the guided mode resonance (GMR) in the system and the robust exciton in the W S 2 monolayer. The dispersive GMR can strongly interact with the nondispersive exciton state by tuning the incident angle, resulting in remarkable Rabi splitting and the emergence of two hybrid polariton bands. The strong GMR–exciton coupling behavior can be well described by the classic oscillator model. The influence of the geometrical parameters on the spectral response is investigated. In addition, we also find that the Rabi splitting is strongly affected by the position of the W S 2 monolayer in the dielectric slab. Our findings provide a simple route for realization of hybrid light–TMDCs interactions, which may inspire related studies on compact, scalable, and easy-to-fabricate TMDC-based devices.

Direct Visualization of Exciton Transport in Defective Few-Layer WS2 by Ultrafast Microscopy.

As defects usually limit the exciton diffusion in 2D transition metal dichalcogenides (TMDCs), the interaction knowledge of defects and exciton transport is crucial for achieving efficient TMDC-based devices. A direct visualization of defect-modulated exciton transport is developed in few-layer WS2 by ultrafast transient absorption microscopy. Atomic-scale defects are introduced by argon plasma treatment and identified by aberration-corrected scanning transmission electron microscopy. Neutral excitons can be captured by defects to form bound excitons in 7.75-17.88 ps, which provide a nonradiative relaxation channel, leading to decreased exciton lifetime and diffusion coefficient. The exciton diffusion length of defective sample has a drastic reduction from 349.44 to 107.40 nm. These spatially and temporally resolved measurements reveal the interaction mechanism between defects and exciton transport dynamics in 2D TMDCs, giving a guideline for designing high-performance TMDC-based devices.

Universal Fermi-Level Pinning in Transition-Metal Dichalcogenides.

Understanding the electron transport through transition-metal dichalcogenide (TMDC)-based semiconductor/metal junctions is vital for the realization of future TMDC-based (opto-)electronic devices. Despite the bonding in TMDCs being largely constrained within the layers, strong Fermi-level pinning (FLP) was observed in TMDC-based devices, reducing the tunability of the Schottky barrier height. We present evidence that metal-induced gap states (MIGS) are the origin for the large FLP similar to conventional semiconductors. A variety of TMDCs (MoSe2, WSe2, WS2, and MoTe2) were investigated using high-spatial-resolution surface characterization techniques, permitting us to distinguish between defected and pristine regions. The Schottky barrier heights on the pristine regions can be explained by MIGS, inducing partial FLP. The FLP strength is further enhanced by disorder-induced gap states induced by transition-metal vacancies or substitutionals at the defected regions. Our findings emphasize the importance of defects on the electron transport properties in TMDC-based devices and confirm the origin of FLP in TMDC-based metal/semiconductor junctions.

Lowering the Schottky Barrier Height by Graphene/Ag Electrodes for High-Mobility MoS2 Field-Effect Transistors.

2D transition metal dichalcogenides (TMDCs) have emerged as promising candidates for post-silicon nanoelectronics owing to their unique and outstanding semiconducting properties. However, contact engineering for these materials to create high-performance devices while adapting for large-area fabrication is still in its nascent stages. In this study, graphene/Ag contacts are introduced into MoS2 devices, for which a graphene film synthesized by chemical vapor deposition (CVD) is inserted between a CVD-grown MoS2 film and a Ag electrode as an interfacial layer. The MoS2 field-effect transistors with graphene/Ag contacts show improved electrical and photoelectrical properties, achieving a field-effect mobility of 35 cm2 V-1 s-1 , an on/off current ratio of 4 × 108 , and a photoresponsivity of 2160 A W-1 , compared to those of devices with conventional Ti/Au contacts. These improvements are attributed to the low work function of Ag and the tunability of graphene Fermi level; the n-doping of Ag in graphene decreases its Fermi level, thereby reducing the Schottky barrier height and contact resistance between the MoS2 and electrodes. This demonstration of contact interface engineering with CVD-grown MoS2 and graphene is a key step toward the practical application of atomically thin TMDC-based devices with low-resistance contacts for high-performance large-area electronics and optoelectronics.

Two-dimensional transition metal dichalcogenides: interface and defect engineering.

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been considered as promising candidates for next generation nanoelectronics. Because of their atomically-thin structure and high surface to volume ratio, the interfaces involved in TMDC-based devices play a predominant role in determining the device performance, such as charge injection/collection at the metal/TMDC interface, and charge carrier trapping at the dielectric/TMDC interface. On the other hand, the crystalline structures of TMDCs are enriched by a variety of intrinsic defects, including vacancies, adatoms, grain boundaries, and substitutional impurities. Customized design and engineering of the interfaces and defects provides an effective way to modulate the properties of TMDCs and finally enhance the device performance. Herein, we summarize and highlight recent advances and state-of-the-art investigations on the interface and defect engineering of TMDCs and their corresponding applications in electronic and optoelectronic devices. Various interface engineering approaches for TMDCs are overviewed, including surface charge transfer doping, TMDC/metal contact engineering, and TMDC/dielectric interface engineering. Subsequently, different types of structural defects in TMDCs are introduced. Defect engineering strategies utilized to modulate the optical and electronic properties of TMDCs, as well as the developed high-performance and functional devices are summarized. Finally, we highlight the challenges and opportunities for interface and defect engineering in TMDC materials for electronics and optoelectronics.

Nanoscale Multilayer Transition-Metal Dichalcogenide Heterostructures: Band Gap Modulation by Interfacial Strain and Spontaneous Polarization.

Using density functional theory calculations, we unveil intriguing electronic properties of nanoscale multilayer transition-metal dichalcogenide (TMDC) heterostructures, (MoX2)n(MoY2)m (X, Y = S, Se or Te). Our results show that the structural stability and electronic band structure of the TMDC heterostructures depend sensitively on the choice of constituent components and their relative thickness. In particular, the electronic band gap can be tuned over a wide range by the intrinsic mismatch strain and spontaneous electrical polarization at the interface of the heterostructures, which suggests desirable design strategies for TMDC-based devices with an easily adjustable band gap. These interfacial effects also make the electronic properties more susceptible to the influence of a bias electric field, which can induce sensitive and considerable changes in the band gap and even produce a semiconductor-metal transition at relatively low electric fields. Such effective electronic band gap engineering via a combination of internal (i.e., the composition and layer thickness) and external (i.e., a bias field) control makes the TMDC-based heterostructures promising candidates for applications in a variety of nanodevices.