MoS2-based Electronic Devices Research Articles

The Contact Properties of Monolayer and Multilayer MoS2-Metal van der Waals Interfaces.

The contact resistance formed between MoS2 and metal electrodes plays a key role in MoS2-based electronic devices. The Schottky barrier height (SBH) is a crucial parameter for determining the contact resistance. However, the SBH is difficult to modulate because of the strong Fermi-level pinning (FLP) at MoS2-metal interfaces. Here, we investigate the FLP effect and the contact types of monolayer and multilayer MoS2-metal van der Waals (vdW) interfaces using density functional theory (DFT) calculations based on Perdew-Burke-Ernzerhof (PBE) level. It has been demonstrated that, compared with monolayer MoS2-metal close interfaces, the FLP effect can be significantly reduced in monolayer MoS2-metal vdW interfaces. Furthermore, as the layer number of MoS2 increases from 1L to 4L, the FLP effect is first weakened and then increased, which can be attributed to the charge redistribution at the MoS2-metal and MoS2-MoS2 interfaces. In addition, the p-type Schottky contact can be achieved in 1L-4L MoS2-Pt, 3L MoS2-Au, and 2L-3L MoS2-Pd vdW interfaces, which is useful for realizing complementary metal oxide semiconductor (CMOS) logic circuits. These findings indicated that the FLP and contact types can be effectively modulated at MoS2-metal vdW interfaces by selecting the layer number of MoS2.

Internal photoemission of electrons from 2D semiconductor/3D metal barrier structures

Understanding the energy alignment of electronic bands, which originate from ultrathin MoS2 layers and metal electrodes attached to them, is crucial for the design of MoS2-based electronic devices. We have applied internal photoemission spectroscopy (IPE) to analyze this alignment. We demonstrate that IPE can yield the barrier heights in the metal/ two-dimensional semiconductor/insulator stacks when the top metal electrode is sufficiently thin for allowing both the photoexcitation of electrons and their transport towards the insulator. The electron barrier at the interface between Al and monolayer (1ML) of MoS2 is estimated at 0.7 eV, and this value explains the experimentally observed attenuated quantum yield contribution from the aluminum. Based on the relative energies of the low-energy threshold position and the Fermi level of aluminum at the interface with the SiO2 insulator, we provide a simple explanation for the observed current photoinjection at the interface between aluminum and 1ML MoS2.

Electrical contacts to few-layer MoS2 with phase-engineering and metal intercalation for tuning the contact performance.

Due to Fermi-level pinning in metal-two-dimensional MoS2 junctions, improving the performance of MoS2-based electrical devices is still under extensive study. The device performance of few-layer MoS2 depends strongly on the number of layers. In this work, via density-functional theory calculations, a comprehensive understanding from the atomistic view was reached for the interlayer interaction between metal and few-layer MoS2 with phase-engineering and intercalation doping, which are helpful for improving the contact performance. These two methods are probed to tune the performance of few-layer MoS2-based field-effect transistors, and both of them can tune the Schottky barrier height. Phase-engineering, which means that the MoS2 layer in contact with metal is converted to the T phase, can transform the Schottky barrier from n- to p-type. Intercalation doping, which takes advantage of annealing and results in metal atom interaction in between MoS2 layers, makes the MoS2 layers become quasi-freestanding and converts the indirect bandgap into direct bandgap. Our atomistic insights help improve the performance of few-layer MoS2-based electronic devices.

Improved low-frequency noise in CVD bilayer MoS2 field-effect transistors

In MoS2 field-effect transistors, the current or voltage fluctuations related to either mobility- or number-dependent relationships are characterized by low-frequency noise. This noise can typically be used to evaluate the application limits of MoS2-based electronic devices. In this work, the low-frequency noise characteristics of single-crystal bilayer MoS2 grown by chemical vapor deposition (CVD) are systematically investigated and found to offer significant performance improvements compared with those based on the monolayer MoS2 channel. At f = 100 Hz, the normalized drain current power spectral density (SI/Id2) is 2.4 × 10−10 Hz−1 and 3.1 × 10−9 Hz−1 for bilayer and monolayer MoS2 transistors, respectively. The 1/f noise behavior can be accurately described by McWhorter's carrier number fluctuation model for both transistor types, suggesting that carrier trapping and de-trapping by dielectric defects is the dominant mechanism of 1/f noise in CVD MoS2 transistors. Furthermore, a minimal WLSI/Id2 of 3.1 × 10−10 μm2/Hz (where W is the gate width and L is the gate length) is achieved at Vbg = 3 V by effectively reducing the contact resistance of bilayer MoS2 transistors using a back-gate voltage. These results demonstrate that CVD bilayer MoS2 is a promising candidate for future large-scale 2D-semiconductor-based electronic applications with improved noise performance.

Patterning of transition metal dichalcogenides catalyzed by surface plasmons with atomic precision

Summary Plasmon-induced charge transfer has drawn considerable interests and spurred rapid developments of photovoltaics and photocatalysis. Various plasmonic metal/transition metal dichalcogenide (TMD) heterostructures have been developed to promote charge separation. For plasmon-induced catalysis, the transformation of TMDs is rare, and the erosion of TMDs has not yet been reported. Here, we report the etching of two-dimensional TMDs by planar surface plasmon polaritons (SPPs). We found that SPPs can etch various TMDs into desired layers and lateral size through controlling the light power and incident direction. In aqueous media, the strong plasmonic coupling at Au/MoS2 interface generates holes in the valence band of MoS2 that can weaken its interlayer interaction. As a synergistic effect, the plasmonic hot electrons produce oxidizing H2O2 to dissolve MoS2 from the top layers. Our results provide a new perspective for understanding the plasmonic coupling at metal-TMD interfaces and a reliable route toward fabricating well-defined TMDs.

The modulation of terahertz photoconductivity in CVD grown n-doped monolayer MoS2 with gas adsorption

The as-grown atomically thin transition metal dichalcogenides (TMDs) usually have extremely large surface-to-volume ratios. Hence, the electrical and optical properties are always affected by the adsorption of atmospheric gases. By using optical pump terahertz (THz) probe spectroscopy, THz photoconductivity dynamics of chemical vapor deposition grown monolayer MoS2 has been investigated in nitrogen, air and oxygen atmospheric environments. Our study reveals that the photoconductivity of MoS2 at THz frequencies is dramatically altered by the adsorption of oxygen. The relaxation dynamics of photoconductivity strongly depends on atmospheres, which is attributed to photo-excited different quasi-particles, such as free charge carriers, excitons and trions. This study highlights the role of oxygen passivation of the photoconductivity in monolayer MoS2, which may have important applications for the design of future MoS2-based electronic devices.

Low-voltage electric-double-layer MoS2 transistor gated via water solution

Two-dimensional (2D) molybdenum disulfide (MoS2) has attracted growing interests due to its intriguing electrical, optical, and scalable properties. Exploring 2D MoS2-based electronic devices which are compatible with the biological systems are of great significance. Herein, a proof-of-concept water-gated multilayer MoS2 transistor is successfully demonstrated by using a side-gated device architecture. Electric-double-layer (EDL) effect is observed in such water-gated multilayer MoS2 transistor. The device exhibits a good performance with a high current on/off ratio of 4 × 103, a small subthreshold swing of 0.27 V/dec, and a low operation voltage of ∼1.5 V, respectively. Furthermore, an ion-contributed quasi-EDL model can be further confirmed by the frequency-dependent capacitance and phase angle measurements. Such merits of water-containing systems coupled with MoS2 opens new opportunities to harness the excellent physical and electrical properties of 2D MoS2 for the potential bioelectronic devices integrated in biological systems for monitoring, diagnostic, and medical applications.

Investigation of CHF3 treatment on the energy band at the MoS2/HfZrO4 heterostructure

The energy band engineering at the multilayer MoS2 (5 nm)/HfZrO4 (15 nm) heterojunction and the effects of CHF3 plasma treatment on the band offset were investigated using x-ray photoelectron spectroscopy. For the MoS2/HfZrO4 sample without CHF3 plasma treatment, the valence band offset is about 1.00 eV and 3.20 eV for the conduction band offset. With CHF3 plasma treatment, the conduction band offset was reduced by 0.37 eV. The band alignment difference is believed to be dominated by the up-shift of the Hf 4f core level, which is consistent with the calculation result that F ions have a strong interaction with Hf atoms. This interesting finding encourages the application of HfZrO4 as gate oxide materials in MoS2-based electronic devices.

Modified MXene: promising electrode materials for constructing Ohmic contacts with MoS2 for electronic device applications.

The development of MoS2-based electronic devices is dependent on finding electrode materials suitable for forming Ohmic contacts with MoS2. For this purpose, we carried out density functional theory and nonequilibrium Green's function calculations to investigate the possibility of using pristine and modified MXene (Ta2C/Ta2CF2/Ta2C(OH)2) monolayers as the electrode materials in such devices. These calculations indicated the formation of chemical bonds at the MoS2/Ta2C interface, and resulting strong orbital hybridization between the MoS2 and Ta2C components, but relatively weak interactions for MoS2/Ta2CF2 and MoS2/Ta2C(OH)2. Ohmic contacts were observed in all three cases. Transport properties were further simulated by modeling two-probe field effect transistors (FETs) with Ta2C/Ta2CF2/Ta2C(OH)2 as electrodes. Interestingly, these simulations indicated the formation of Ohmic contacts between Ta2CF2/Ta2C(OH)2 electrodes and the channel, but an n-type Schottky barrier for the Ta2C electrode. Furthermore, we found the resistance of the FET based on MoS2/Ta2C(OH)2 to be half of that based on MoS2/Ta2CF2. The results of our study not only revealed promising electrode materials for forming full Ohmic contacts with MoS2 monolayers in FET devices, but also validated the effective role of a small-molecule fragment as a buffer layer in realizing Ohmic contacts between metal and semiconductor.

Effect of post-annealing on sputtered MoS2 films

Typical routes for fabricating MoS2-based electronic devices rely on the transfer of as-prepared flakes to target substrates, which is incompatible with conventional device fabrication methods. In this work we investigated the preparation of MoS2 films by magnetron sputtering. By subjecting room-temperature sputtered MoS2 films to post-annealing at mild conditions (450°C in a nitrogen flow), crystalline MoS2 films were formed. To demonstrate the compatibility of the technique with typical device fabrication processes, MoS2 was prepared on epitaxial magnetic oxide films of La0.7Sr0.3MnO3, and the magnetic behavior of the films were unaffected by the post-annealing process. This work demonstrates the possibility of fabricating electronic and spintronic devices based on continuous MoS2 films prepared by sputtering deposition.

Defect Dominated Charge Transport and Fermi Level Pinning in MoS2/Metal Contacts.

Understanding the electronic contact between molybdenum disulfide (MoS2) and metal electrodes is vital for the realization of future MoS2-based electronic devices. Natural MoS2 has the drawback of a high density of both metal and sulfur defects and impurities. We present evidence that subsurface metal-like defects with a density of ∼1011 cm–2 induce negative ionization of the outermost S atom complex. We investigate with high-spatial-resolution surface characterization techniques the effect of these defects on the local conductance of MoS2. Using metal nanocontacts (contact area < 6 nm2), we find that subsurface metal-like defects (and not S-vacancies) drastically decrease the metal/MoS2 Schottky barrier height as compared to that in the pristine regions. The magnitude of this decrease depends on the contact metal. The decrease of the Schottky barrier height is attributed to strong Fermi level pinning at the defects. Indeed, this is demonstrated in the measured pinning factor, which is equal to ∼0.1 at defect locations and ∼0.3 at pristine regions. Our findings are in good agreement with the theoretically predicted values. These defects provide low-resistance conduction paths in MoS2-based nanodevices and will play a prominent role as the device junction contact area decreases in size.

MoS2-graphene in-plane contact for high interfacial thermal conduction

Recent studies showed that the in-plane and inter-plane thermal conductivities of two-dimensional (2D) MoS2 are low, posing a significant challenge in heat management in MoS2-based electronic devices. To address this challenge, we design the interfaces between MoS2 and graphene by fully utilizing graphene, a 2D material with an ultra-high thermal conduction. We first perform ab initio atomistic simulations to understand the bonding nature and structure stability of the interfaces. Our results show that the designed interfaces, which are found to be connected together by strong covalent bonds between Mo and C atoms, are energetically stable. We then perform molecular dynamics simulations to investigate the interfacial thermal conductance. It is found surprisingly that the interface thermal conductance is high, comparable to that of graphene-metal covalent-bonded interfaces. Importantly, each interfacial Mo-C bond serves as an independent thermal channel, enabling the modulation of interfacial thermal conductance by controlling Mo vacancy concentration at the interface. The present work provides a viable route for heat management in MoS2 based electronic devices.

Thermal conduction across the one-dimensional interface between a MoS2 monolayer and metal electrode

The thermal conductance across the one-dimensional (1D) interface between a MoS2 monolayer and Au electrode (edge-contact) has been investigated using molecular dynamics simulations. Although the thermal conductivity of monolayer MoS2 is 2–3 orders of magnitude lower than that of graphene, the covalent bonds formed at the interface enable interfacial thermal conductance (ITC) that is comparable to that of a graphene–metal interface. Each covalent bond at the interface serves as an independent channel for thermal conduction, allowing ITC to be tuned linearly by changing the interfacial bond density (controlling S vacancies). In addition, different Au surfaces form different bonding configurations, causing large ITC variations. Interestingly, the S vacancies in the central region of MoS2 only slightly affect the ITC, which can be explained by a mismatch of the phonon vibration spectra. Further, at room temperature, ITC is primarily dominated by phonon transport, and electron–phonon coupling plays a negligible role. These results not only shed light on the phonon transport mechanisms across 1D metal–MoS2 interfaces, but also provide guidelines for the design and optimization of such interfaces for thermal management in MoS2-based electronic devices.

Direct Growth of Single- and Few-Layer MoS2 on h-BN with Preferred Relative Rotation Angles.

Monolayer molybdenum disulfide (MoS2) is a promising two-dimensional direct-bandgap semiconductor with potential applications in atomically thin and flexible electronics. An attractive insulating substrate or mate for MoS2 (and related materials such as graphene) is hexagonal boron nitride (h-BN). Stacked heterostructures of MoS2 and h-BN have been produced by manual transfer methods, but a more efficient and scalable assembly method is needed. Here we demonstrate the direct growth of single- and few-layer MoS2 on h-BN by chemical vapor deposition (CVD) method, which is scalable with suitably structured substrates. The growth mechanisms for single-layer and few-layer samples are found to be distinct, and for single-layer samples low relative rotation angles (<5°) between the MoS2 and h-BN lattices prevail. Moreover, MoS2 directly grown on h-BN maintains its intrinsic 1.89 eV bandgap. Our CVD synthesis method presents an important advancement toward controllable and scalable MoS2-based electronic devices.

Optics, mechanics, and energetics of two-dimensional MoS2 nanostructures from a theoretical perspective.

CONSPECTUS: Nanostructures based on molybdenum disulfide (MoS2) are by far the most common and well-studied systems among two-dimensional (2D) semiconducting materials. Although still being characterized as a "promising material", catalytic activity of MoS2 nanostructures has been found, and applications in lubrication processes are pursued. Because exfoliation techniques have improved over the past years, monolayer MoS2 is easily at hand; thus, experimental studies on its electronic properties and applicability are in scientific focus, and some MoS2-based electronic devices have been reported already. Additionally, the improvement of atomic force microscopy led to nanoindentation experiments, in which the exceptional mechanical properties of MoS2 could be confirmed. In this Account, we review recent results from density-functional based calculations on several MoS2-based nanostructures; we have chosen to follow several experimental routes focusing on different nanostructures and their specific properties. MoS2-based triangular nanoflakes are systems that are experimentally well described and studied with a special focus on their optical absorption. The interpretation of our calculations fits well to the experimental picture: the absorption peaks in the visible light range show a quantum-confinement effect; they originate from excitations into the edge states. Additionally, delocalized metallic-like states are present close to the Fermi level, which do not contribute to photoabsorption in the visible range. Additionally, nanoindentation experiments have been simulated to obtain mechanical properties of the MoS2 material and to study the influence of deformation on the system's electronics. In these molecular-dynamics simulations, a tip penetrates a MoS2 monolayer, and the obtained Young's modulus and breaking stress agree very well with experimentally obtained values. Whereas the structural properties, such as bond lengths and layer contraction, vary locally differently upon indentation, the electronic structure in terms of the density of states, the gap between occupied and unoccupied states, or the quantum transport change only slightly. The robustness of the material with respect to electronic and mechanical properties makes monolayer MoS2 special. However, it is important to note that this robustness refers to a local disturbance through deformation and still seems to be dependent on the defect concentration. Finally, we present a comparison of the thermodynamic stabilities of different MoS2-based nanostructures with a focus on nanoflakes, fullerene-like nanooctahedra, and smaller Chevrel-type and non-Chevrel-type clusters (nanowires). All studied systems are stable in comparison to MoS2, Mo bulk, and the S8 crown, but only the studied nanoflakes and nanowires show specific stoichiometries, either sulfur-rich or sulfur-poor, whereas the nanooctahedra may adopt both. From the thermodynamic stabilities, it should be possible to deliberately choose specific nanostructures by thoughtful choices of the synthesis conditions. In conclusion, we present in this Account exceptional properties of MoS2-based nanostructures studied by means of density-functional theory. The focus lies on optical absorption in the visible range observed in triangular nanoflakes, which originate in the system's edge states, the robustness of monolayer MoS2 with respect to punctual loads regarding both mechanical and electronic properties, and the thermodynamic stability of most studied MoS2-based nanosystems revealing a correlation between composition and preferred morphology, particularly for 2D systems.

Graphene oxide as a promising hole injection layer for MoS₂-based electronic devices.

The excellent physical and semiconducting properties of transition metal dichalcogenide (TMDC) monolayers make them promising materials for many applications. The TMDC monolayer MoS2 has gained significant attention as a channel material for next-generation transistors. However, while n-type single-layer MoS2 devices can be made with relative ease, fabrication of p-type transistors remains a challenge as the Fermi-level of elemental metals used as contacts are pinned close to the conduction band leading to large p-type Schottky barrier heights (SBH). Here, we propose the utilization of graphene oxide (GO) as an efficient hole injection layer for single-layer MoS2-based electronic and optoelectronic devices. Using first-principles computations, we demonstrate that GO forms a p-type contact with monolayer MoS2, and that the p-type SBH can be made smaller by increasing the oxygen concentration and the fraction of epoxy functional groups in GO. Our analysis shows that this is possible due to the high work function of GO and the relatively weak Fermi-level pinning at the MoS2/GO interfaces compared to traditional MoS2/metal systems (common metals are Ag, Al, Au, Ir, Pd, Pt). The combination of easy-to-fabricate and inexpensive GO with MoS2 could be promising for the development of hybrid all-2D p-type electronic and optoelectronic devices on flexible substrates.

Electric Stress-Induced Threshold Voltage Instability of Multilayer MoS2 Field Effect Transistors

We investigated the gate bias stress effects of multilayered MoS2 field effect transistors (FETs) with a back-gated configuration. The electrical stability of the MoS2 FETs can be significantly influenced by the electrical stress type, relative sweep rate, and stress time in an ambient environment. Specifically, when a positive gate bias stress was applied to the MoS2 FET, the current of the device decreased and its threshold shifted in the positive gate bias direction. In contrast, with a negative gate bias stress, the current of the device increased and the threshold shifted in the negative gate bias direction. The gate bias stress effects were enhanced when a gate bias was applied for a longer time or when a slower sweep rate was used. These phenomena can be explained by the charge trapping due to the adsorption or desorption of oxygen and/or water on the MoS2 surface with a positive or negative gate bias, respectively, under an ambient environment. This study will be helpful in understanding the electrical-stress-induced instability of the MoS2-based electronic devices and will also give insight into the design of desirable devices for electronics applications.

Oxygen environmental and passivation effects on molybdenum disulfide field effect transistors

We investigated the effects of passivation on the electrical characteristics of molybdenum disulfide (MoS2) field effect transistors (FETs) under nitrogen, vacuum, and oxygen environments. When the MoS2 FETs were exposed to oxygen, the on-current decreased and the threshold voltage shifted in the positive gate bias direction as a result of electrons being trapped by the adsorbed oxygen at the MoS2 surface. In contrast, the electrical properties of the MoS2 FETs changed only slightly in the different environments when a passivation layer was created using polymethyl methacrylate (PMMA). Specifically, the carrier concentration of unpassivated devices was reduced to 6.5 × 1015 cm−2 in oxygen from 16.3 × 1015 cm−2 in nitrogen environment. However, in PMMA-passivated devices, the carrier concentration remained nearly unchanged in the range of 1–3 × 1015 cm−2 regardless of the environment. Our study suggests that surface passivation is important for MoS2-based electronic devices.