Gap‐Mode Surface‐Plasmon‐Enhanced Photoluminescence and Photoresponse of MoS2

2D materials hold great potential for designing novel electronic and optoelectronic devices. However, 2D material can only absorb limited incident light. As a representative 2D semiconductor, monolayer MoS₂ can only absorb up to 10% of the incident light in the visible, which is not sufficient to achieve a high optical‐to‐electrical conversion efficiency. To overcome this shortcoming, a “gap‐mode” plasmon‐enhanced monolayer MoS₂ fluorescent emitter and photodetector is designed by squeezing the light‐field into Ag shell‐isolated nanoparticles–Au film gap, where the confined electromagnetic field can interact with monolayer MoS₂. With this gap‐mode plasmon‐enhanced configuration, a 110‐fold enhancement of photoluminescence intensity is achieved, exceeding values reached by other plasmon‐enhanced MoS₂ fluorescent emitters. In addition, a gap‐mode plasmon‐enhanced monolayer MoS₂ photodetector with an 880% enhancement in photocurrent and a responsivity of 287.5 A W^?1 is demonstrated, exceeding previously reported plasmon‐enhanced monolayer MoS₂ photodetectors.     

MoS2 Negative‐Capacitance Field‐Effect Transistors with Subthreshold Swing below the Physics Limit

The Boltzmann distribution of electrons induced fundamental barrier prevents subthreshold swing (SS) from less than 60 mV dec^‐1 at room temperature, leading to high energy consumption of MOSFETs. Herein, it is demonstrated that an aggressive introduction of the negative capacitance (NC) effect of ferroelectrics can decisively break the fundamental limit governed by the “Boltzmann tyranny”. Such MoS₂ negative‐capacitance field‐effect transistors (NC‐FETs) with self‐aligned top‐gated geometry demonstrated here pull down the SS value to 42.5 mV dec^‐1, and simultaneously achieve superior performance of a transconductance of 45.5 μS μm and an on/off ratio of 4 × 10⁶ with channel length less than 100 nm. Furthermore, the inserted HfO₂ layer not only realizes a stable NC gate stack structure, but also prevents the ferroelectric P(VDF‐TrFE) from fatigue with robust stability. Notably, the fabricated MoS₂ NC‐FETs are distinctly different from traditional MOSFETs. The on‐state current increases as the temperature decreases even down to 20 K, and the SS values exhibit nonlinear dependence with temperature due to the implementation of the ferroelectric gate stack. The NC‐FETs enable fundamental applications through overcoming the Boltzmann limit in nanoelectronics and open up an avenue to low‐power transistors needed for many exciting long‐endurance portable consumer products.     

Impact of H‐Doping on n‐Type TMD Channels for Low‐Temperature Band‐Like Transport

Band‐like transport behavior of H‐doped transition metal dichalcogenide (TMD) channels in field effect transistors (FET) is studied by conducting low‐temperature electrical measurements, where MoTe₂, WSe₂, and MoS₂ are chosen for channels. Doped with H atoms through atomic layer deposition, those channels show strong n‐type conduction and their mobility increases without losing on‐state current as the measurement temperature decreases. In contrast, the mobility of unintentionally (naturally) doped TMD FETs always drops at low temperatures whether they are p‐ or n‐type. Density functional theory calculations show that H‐doped MoTe₂, WSe₂, and MoS₂ have Fermi levels above conduction band edge. It is thus concluded that the charge transport behavior in H‐doped TMD channels is metallic showing band‐like transport rather than thermal hopping. These results indicate that H‐doped TMD FETs are practically useful even at low‐temperature ranges.     

Graphene‐Contacted Ultrashort Channel Monolayer MoS2 Transistors

2D semiconductors are promising channel materials for field‐effect transistors (FETs) with potentially strong immunity to short‐channel effects (SCEs). In this paper, a grain boundary widening technique is developed to fabricate graphene electrodes for contacting monolayer MoS₂. FETs with channel lengths scaling down to ≈4 nm can be realized reliably. These graphene‐contacted ultrashort channel MoS₂ FETs exhibit superior performances including the nearly Ohmic contacts and excellent immunity to SCEs. This work provides a facile route toward the fabrication of various 2D material‐based devices for ultrascaled electronics.     

Engineering Chemically Active Defects in Monolayer MoS2 Transistors via Ion‐Beam Irradiation and Their Healing via Vapor Deposition of Alkanethiols

Irradiation of 2D sheets of transition metal dichalcogenides with ion beams has emerged as an effective approach to engineer chemically active defects in 2D materials. In this context, argon‐ion bombardment has been utilized to introduce sulfur vacancies in monolayer molybdenum disulfide (MoS₂). However, a detailed understanding of the effects of generated defects on the functional properties of 2D MoS₂ is still lacking. In this work, the correlation between critical electronic device parameters and the density of sulfur vacancies is systematically investigated through the fabrication and characterization of back‐gated monolayer MoS₂ field‐effect transistors (FETs) exposed to a variable fluence of low‐energy argon ions. The electrical properties of pristine and ion‐irradiated FETs can be largely improved/recovered by exposing the devices to vapors of short linear thiolated molecules. Such a solvent‐free chemical treatment—carried out strictly under inert atmosphere—rules out secondary healing effects induced by oxygen or oxygen‐containing molecules. The results provide a guideline to design monolayer MoS₂ optoelectronic devices with a controlled density of sulfur vacancies, which can be further exploited to introduce ad hoc molecular functionalities by means of thiol chemistry approaches.     

SnSe/MoS2 van der Waals Heterostructure Junction Field‐Effect Transistors with Nearly Ideal Subthreshold Slope

The minimization of the subthreshold swing (SS) in transistors is essential for low‐voltage operation and lower power consumption, both critical for mobile devices and internet of things (IoT) devices. The conventional metal‐oxide‐semiconductor field‐effect transistor requires sophisticated dielectric engineering to achieve nearly ideal SS (60 mV dec^?1 at room temperature). However, another type of transistor, the junction field‐effect transistor (JFET) is free of dielectric layer and can reach the theoretical SS limit without complicated dielectric engineering. The construction of a 2D SnSe/MoS₂ van der Waals (vdW) heterostructure‐based JFET with nearly ideal SS is reported. It is shown that the SnSe/MoS₂ vdW heterostructure exhibits excellent p–n diode rectifying characteristics with low saturate current. Using the SnSe as the gate and MoS₂ as the channel, the SnSe/MoS₂ vdW heterostructure exhibit well‐behavioured n‐channel JFET characteristics with a small pinch‐off voltage V_P of ?0.25 V, nearly ideal subthreshold swing SS of 60.3 mV dec^?1 and high ON/OFF ratio over 10⁶, demonstrating excellent electronic performance especially in the subthreshold regime.     

A Fermi‐Level‐Pinning‐Free 1D Electrical Contact at the Intrinsic 2D MoS2–Metal Junction

Currently 2D crystals are being studied intensively for use in future nanoelectronics, as conventional semiconductor devices face challenges in high power consumption and short channel effects when scaled to the quantum limit. Toward this end, achieving barrier‐free contact to 2D semiconductors has emerged as a major roadblock. In conventional contacts to bulk metals, the 2D semiconductor Fermi levels become pinned inside the bandgap, deviating from the ideal Schottky–Mott rule and resulting in significant suppression of carrier transport in the device. Here, MoS₂ polarity control is realized without extrinsic doping by employing a 1D elemental metal contact scheme. The use of high‐work‐function palladium (Pd) or gold (Au) enables a high‐quality p‐type dominant contact to intrinsic MoS₂, realizing Fermi level depinning. Field‐effect transistors (FETs) with Pd edge contact and Au edge contact show high performance with the highest hole mobility reaching 330 and 432 cm² V^?1 s^?1 at 300 K, respectively. The ideal Fermi level alignment allows creation of p‐ and n‐type FETs on the same intrinsic MoS₂ flake using Pd and low‐work‐function molybdenum (Mo) contacts, respectively. This device acts as an efficient inverter, a basic building block for semiconductor integrated circuits, with gain reaching 15 at V_D = 5 V.     

Enhanced Field‐Emission Behavior of Layered MoS2 Sheets

Field emission studies are reported for the first time on layered MoS₂ sheets at the base pressure of ～1 × 10^?8 mbar. The turn‐on field required to draw a field emission current density of 10 μA/cm² is found to be 3.5 V/μm for MoS₂ sheets. The turn‐on values are found to be significantly lower than the reported MoS₂ nanoflowers, graphene, and carbon nanotube‐based field emitters due to the high field enhancement factor (～1138) associated with nanometric sharp edges of MoS₂ sheet emitter surface. The emission current–time plots show good stability over a period of 3 h. Owing to the low turn‐on field and planar (sheetlike) structure, the MoS₂ could be utilized for future vacuum microelectronics/nanoelectronic and flat panel display applications.     

Contact‐Engineered Electrical Properties of MoS2 Field‐Effect Transistors via Selectively Deposited Thiol‐Molecules

Although 2D molybdenum disulfide (MoS₂) has gained much attention due to its unique electrical and optical properties, the limited electrical contact to 2D semiconductors still impedes the realization of high‐performance 2D MoS₂‐based devices. In this regard, many studies have been conducted to improve the carrier‐injection properties by inserting functional paths, such as graphene or hexagonal boron nitride, between the electrodes and 2D semiconductors. The reported strategies, however, require relatively time‐consuming and low‐yield transfer processes on sub‐micrometer MoS₂ flakes. Here, a simple contact‐engineering method is suggested, introducing chemically adsorbed thiol‐molecules as thin tunneling barriers between the metal electrodes and MoS₂ channels. The selectively deposited thiol‐molecules via the vapor‐deposition process provide additional tunneling paths at the contact regions, improving the carrier‐injection properties with lower activation energies in MoS₂ field‐effect transistors. Additionally, by inserting thiol‐molecules at the only one contact region, asymmetric carrier‐injection is feasible depending on the temperature and gate bias.     

Controllable,Wide‐Ranging n‐Doping and p‐Doping of Monolayer Group 6 Transition‐Metal Disulfides and Diselenides

Developing processes to controllably dope transition‐metal dichalcogenides (TMDs) is critical for optical and electrical applications. Here, molecular reductants and oxidants are introduced onto monolayer TMDs, specifically MoS₂, WS₂, MoSe₂, and WSe₂. Doping is achieved by exposing the TMD surface to solutions of pentamethylrhodocene dimer as the reductant (n‐dopant) and “Magic Blue,” [N(C₆H₄‐p‐Br)₃]SbCl₆, as the oxidant (p‐dopant). Current–voltage characteristics of field‐effect transistors show that, regardless of their initial transport behavior, all four TMDs can be used in either p‐ or n‐channel devices when appropriately doped. The extent of doping can be controlled by varying the concentration of dopant solutions and treatment time, and, in some cases, both nondegenerate and degenerate regimes are accessible. For all four TMD materials, the photoluminescence intensity; for all four materials the PL intensity is enhanced with p‐doping but reduced with n‐doping. Raman and X‐ray photoelectron spectroscopy (XPS) also provide insight into the underlying physical mechanism by which the molecular dopants react with the monolayer. Estimates of changes of carrier density from electrical, PL, and XPS results are compared. Overall a simple and effective route to tailor the electrical and optical properties of TMDs is demonstrated.     

A Novel and Facile Route to Synthesize Atomic‐Layered MoS2 Film for Large‐Area Electronics

High‐quality and large‐area molybdenum disulfide (MoS₂) thin film is highly desirable for applications in large‐area electronics. However, there remains a challenge in attaining MoS₂ film of reasonable crystallinity due to the absence of appropriate choice and control of precursors, as well as choice of suitable growth substrates. Herein, a novel and facile route is reported for synthesizing few‐layered MoS₂ film with new precursors via chemical vapor deposition. Prior to growth, an aqueous solution of sodium molybdate as the molybdenum precursor is spun onto the growth substrate and dimethyl disulfide as the liquid sulfur precursor is supplied with a bubbling system during growth. To supplement the limiting effect of Mo (sodium molybdate), a supplementary Mo is supplied by dissolving molybdenum hexacarbonyl (Mo(CO)₆) in the liquid sulfur precursor delivered by the bubbler. By precisely controlling the amounts of precursors and hydrogen flow, full coverage of MoS₂ film is readily achievable in 20 min. Large‐area MoS₂ field effect transistors (FETs) fabricated with a conventional photolithography have a carrier mobility as high as 18.9 cm² V^?1 s^?1, which is the highest reported for bottom‐gated MoS₂‐FETs fabricated via photolithography with an on/off ratio of ≈10⁵ at room temperature.     

Gram‐Scale Aqueous Synthesis of Stable Few‐Layered 1T‐MoS2: Applications for Visible‐Light‐Driven Photocatalytic Hydrogen Evolution

Most recently, much attention has been devoted to 1T phase MoS₂ because of its distinctive phase‐engineering nature and promising applications in catalysts, electronics, and energy storage devices. While alkali metal intercalation and exfoliation methods have been well developed to realize unstable 1T‐MoS₂, but the aqueous synthesis for producing stable metallic phase remains big challenging. Herein, a new synthetic protocol is developed to mass‐produce colloidal metallic 1T‐MoS₂ layers highly stabilized by intercalated ammonium ions (abbreviated as N‐MoS₂). In combination with density functional calculations, the X‐ray diffraction pattern and Raman spectra elucidate the excellent stability of metallic phase. As clearly depicted by high‐angle annular dark‐field imaging in an aberration‐corrected scanning transmission electron microscope and extended X‐ray absorption fine structure, the N‐MoS₂ exhibits a distorted octahedral structure with a 2a ₀ × a ₀ basal plane superlattice and 2.72 Å Mo–Mo bond length. In a proof‐of‐concept demonstration for the obtained material's applications, highly efficient photocatalytic activity is achieved by simply hybridizing metallic N‐MoS₂ with semiconducting CdS nanorods due to the synergistic effect. As a direct outcome, this CdS:N‐MoS₂ hybrid shows giant enhancement of hydrogen evolution rate, which is almost 21‐fold higher than pure CdS and threefold higher than corresponding annealed CdS:2H‐MoS₂.     

Phosphorus‐Mediated MoS2 Nanowires as a High‐Performance Electrode Material for Quasi‐Solid‐State Sodium‐Ion Intercalation Supercapacitors

Molybdenum disulfide (MoS₂) is a promising electrode material for electrochemical energy storage owing to its high theoretical specific capacity and fascinating 2D layered structure. However, its sluggish kinetics for ionic diffusion and charge transfer limits its practical applications. Here, a promising strategy is reported for enhancing the Na⁺‐ion charge storage kinetics of MoS₂ for supercapacitors. In this strategy, electrical conductivity is enhanced and the diffusion barrier of Na⁺ ion is lowered by a facile phosphorus‐doping treatment. Density functional theory results reveal that the lowest energy barrier of dilute Na‐vacancy diffusion on P‐doped MoS₂ (0.11 eV) is considerably lower than that on pure MoS₂ (0.19 eV), thereby signifying a prominent rate performance at high Na intercalation stages upon P‐doping. Moreover, the Na‐vacancy diffusion coefficient of the P‐doped MoS₂ at room temperatures can be enhanced substantially by approximately two orders of magnitude (10^?6–10^?4 cm² s^?1) compared with pure MoS₂. Finally, the quasi‐solid‐state asymmetrical supercapacitor assembled with P‐doped MoS₂ and MnO₂, as the positive and negative electrode materials, respectively, exhibits an ultrahigh energy density of 67.4 W h kg^?1 at 850 W kg^?1 and excellent cycling stability with 93.4% capacitance retention after 5000 cycles at 8 A g^?1.     

Epitaxial Single‐Layer MoS2 on GaN with Enhanced Valley Helicity

Engineering the substrate of 2D transition metal dichalcogenides can couple the quasiparticle interaction between the 2D material and substrate, providing an additional route to realize conceptual quantum phenomena and novel device functionalities, such as realization of a 12‐time increased valley spitting in single‐layer WSe₂ through the interfacial magnetic exchange field from a ferromagnetic EuS substrate, and band‐to‐band tunnel field‐effect transistors with a subthreshold swing below 60 mV dec⁻¹ at room temperature based on bilayer n‐MoS₂ and heavily doped p‐germanium, etc. Here, it is demonstrated that epitaxially grown single‐layer MoS₂ on a lattice‐matched GaN substrate, possessing a type‐I band alignment, exhibits strong substrate‐induced interactions. The phonons in GaN quickly dissipate the energy of photogenerated carriers through electron–phonon interaction, resulting in a short exciton lifetime in the MoS₂/GaN heterostructure. This interaction enables an enhanced valley helicity at room temperature (0.33 ± 0.05) observed in both steady‐state and time‐resolved circularly polarized photoluminescence measurements. The findings highlight the importance of substrate engineering for modulating the intrinsic valley carriers in ultrathin 2D materials and potentially open new paths for valleytronics and valley‐optoelectronic device applications.     

Enhanced Photocarrier Generation with Selectable Wavelengths by M‐Decorated‐CuInS2 Nanocrystals (M = Au and Pt) Synthesized in a Single Surfactant Process on MoS2 Bilayers

A facile approach for the synthesis of Au‐ and Pt‐decorated CuInS₂ nanocrystals (CIS NCs) as sensitizer materials on the top of MoS₂ bilayers is demonstrated. A single surfactant (oleylamine) is used to prepare such heterostructured noble metal decorated CIS NCs from the pristine CIS. Such a feasible way to synthesize heterostructured noble metal decorated CIS NCs from the single surfactant can stimulate the development of the functionalized heterostructured NCs in large scale for practical applications such as solar cells and photodetectors. Photodetectors based on MoS₂ bilayers with the synthesized nanocrystals display enhanced photocurrent, almost 20–40 times higher responsivity and the On/Off ratio is enlarged one order of magnitude compared with the pristine MoS₂ bilayers‐based photodetectors. Remarkably, by using Pt‐ or Au‐decorated CIS NCs, the photocurrent enhancement of MoS₂ photodetectors can be tuned between blue (405 nm) to green (532 nm). The strategy described here acts as a perspective to significantly improve the performance of MoS₂‐based photodetectors with the controllable absorption wavelengths in the visible light range, showing the feasibility of the possible color detection.     

Penne‐Like MoS2/Carbon Nanocomposite as Anode for Sodium‐Ion‐Based Dual‐Ion Battery

The dual‐ion battery (DIB) system has attracted great attention owing to its merits of low cost, high energy, and environmental friendliness. However, the DIBs based on sodium‐ion electrolytes are seldom reported due to the lack of appropriate anode materials for reversible Na⁺ insertion/extraction. Herein, a new sodium‐ion based DIB named as MoS₂/C‐G DIB using penne‐like MoS₂/C nanotube as anode and expanded graphite as cathode is constructed and optimized for the first time. The hierarchical MoS₂/C nanotube provides expanded (002) interlayer spacing of 2H‐MoS₂, which facilitates fast Na⁺ insertion/extraction reaction kinetics, thus contributing to improved DIB performance. The MoS₂/C‐G DIB delivers a reversible capacity of 65 mA h g^?1 at 2 C in the voltage window of 1.0–4.0 V, with good cycling performance for 200 cycles and 85% capacity retention, indicating the feasibility of potential applications for sodium‐ion based DIBs.     

Triboiontronic Transistor of MoS2

Electric double layers (EDLs) formed in electrolyte‐gated field‐effect transistors (FETs) induce an extremely large local electric field that gives a highly efficient charge carrier control in the semiconductor channel. To achieve highly efficient triboelectric potential gating on the FET and explore diversified applications of electric double layer FETs (EDL‐FETs), a triboiontronic transistor is proposed to bridge triboelectric potential modulation and ion‐controlled semiconductor devices. Utilizing the triboelectric potential instead of applying an external gate voltage, the triboiontronic MoS₂ transistor is efficiently operated owing to the formation of EDLs in the ion‐gel dielectric layer. The operation mechanism of the triboiontronic transistor is proposed, and high current on/off ratio over 10⁷, low threshold value (75 μm), and steep switching properties (20 µm dec^?1) are achieved. A triboiontronic logic inverter with desirable gain (8.3 V mm^?1), low power consumption, and high stability is also demonstrated. This work presents a low‐power‐consuming, active, and a general approach to efficiently modulate semiconductor devices through mechanical instructions, which has great potential in human–machine interaction, electronic skin, and intelligent wearable devices. The proposed triboiontronics utilize ion migration and arrangement triggered by mechanical stimuli to control electronic properties, which are ready to deliver new interdisciplinary research directions.     

MoS2/Rubrene van der Waals Heterostructure: Toward Ambipolar Field‐Effect Transistors and Inverter Circuits

2D transition metal dichalcogenides are promising channel materials for the next‐generation electronic device. Here, vertically 2D heterostructures, so called van der Waals solids, are constructed using inorganic molybdenum sulfide (MoS₂) few layers and organic crystal – 5,6,11,12‐tetraphenylnaphthacene (rubrene). In this work, ambipolar field‐effect transistors are successfully achieved based on MoS₂ and rubrene crystals with the well balanced electron and hole mobilities of 1.27 and 0.36 cm² V^?1 s^?1, respectively. The ambipolar behavior is explained based on the band alignment of MoS₂ and rubrene. Furthermore, being a building block, the MoS₂/rubrene ambipolar transistors are used to fabricate CMOS (complementary metal oxide semiconductor) inverters that show good performance with a gain of 2.3 at a switching threshold voltage of ?26 V. This work paves a way to the novel organic/inorganic ultrathin heterostructure based flexible electronics and optoelectronic devices.     

Electrically Pumped White‐Light‐Emitting Diodes Based on Histidine‐Doped MoS2 Quantum Dots

MoS₂ quantum dots (QDs)‐based white‐light‐emitting diodes (QD‐WLEDs) are designed, fabricated, and demonstrated. The highly luminescent, histidine‐doped MoS₂ QDs synthesized by microwave induced fragmentation of 2D MoS₂ nanoflakes possess a wide distribution of available electronic states as inferred from the pronounced excitation‐wavelength‐dependent emission properties. Notably, the histidine‐doped MoS₂ QDs show a very strong emission intensity, which exceeds seven times of magnitude larger than that of pristine MoS₂ QDs. The strongly enhanced emission is mainly attributed to nitrogen acceptor bound excitons and passivation of defects by histidine‐doping, which can enhance the radiative recombination drastically. The enabled electroluminescence (EL) spectra of the QD‐WLEDs with the main peak around 500 nm are found to be consistent with the photoluminescence spectra of the histidine‐doped MoS₂ QDs. The enhanced intensity of EL spectra with the current increase shows the stability of histidine‐doped MoS₂ based QD‐WLEDs. The typical EL spectrum of the novel QD‐WLEDs has a Commission Internationale de l'Eclairage chromaticity coordinate of (0.30, 0.36) exhibiting an intrinsic broadband white‐light emission. The unprecedented and low‐toxicity QD‐WLEDs based on a single light‐emitting material can serve as an excellent alternative for using transition metal dichalcogenides QDs as next generation optoelectronic devices.     

Giant Enhancements of Perpendicular Magnetic Anisotropy and Spin‐Orbit Torque by a MoS2 Layer

2D transition metal dichalcogenides have attracted much attention in the field of spintronics due to their rich spin‐dependent properties. The promise of highly compact and low‐energy‐consumption spin‐orbit torque (SOT) devices motivates the search for structures and materials that can satisfy the requirements of giant perpendicular magnetic anisotropy (PMA) and large SOT simultaneously in SOT‐based magnetic memory. Here, it is demonstrated that PMA and SOT in a heavy metal/transition metal ferromagnet structure, Pt/[Co/Ni]₂, can be greatly enhanced by introducing a molybdenum disulfide (MoS₂) underlayer. According to first‐principles calculation and X‐ray absorption spectroscopy (XAS), the enhancement of the PMA is ascribed to the modification of the orbital hybridization at the interface of Pt/Co due to MoS₂. The enhancement of SOT by the role played by MoS₂ is explained, which is strongly supported by the identical behavior of SOT and PMA as a function of Pt thickness. This work provides new possibilities to integrate 2D materials into promising spintronics devices.