2D MoS2 Layers Research Articles

Facile Synthesis of Vertically Aligned MoS2 Nanosheets at Ambient Pressure

AbstractVertically aligned 2D molybdenum disulfide (MoS2) nanosheets are grown directly on SiO2/Si substrate using an ordinary tubular furnace under 850 °C temperature and atmospheric pressure condition. To achieve high‐quality vertically aligned 2D MoS2, the amount of precursor material, i.e., molybdenum trioxide (MoO3) powder and sulfur (S), is varied, keeping the other parameters such as temperature and carrier gas flow rate constant. The Raman spectroscopy confirms the formation of 2D MoS2 layers and it illustrates that as‐grown MoS2 is in few‐layer forms with good crystallinity. The Raman spectra identifies the best quality 2D MoS2. The topographical and morphological studies of MoS2 carried out by atomic force microscope (AFM) and field effect scanning microscope (FESEM) reveal that as‐synthesized MoS2 is vertically aligned. X‐ray diffraction and energy dispersive spectroscopy (EDS) are carried out in order to identify the phase and elements in the product. In the present work, the emphasis is given on the vertical alignment rather than the thickness of 2D MoS2. Finally, it is demonstrated that vertically aligned 2D MoS2 can be grown simply on SiO2/Si substrate using a simple ordinary tubular furnace under atmospheric pressure condition by varying the amount of MoO3 and S.

Stable performance of Li-S battery: Engineering of Li2S smart cathode by reduction of multilayer graphene-embedded 2D-MoS2

Lithium-sulfur (Li–S) batteries are considered promising candidates for next-generation energy storage devices due to their ultrahigh theoretical gravimetric energy density, cost-effectiveness, and environmental friendliness. However, the application of Li–S batteries remains challenging; mainly due to a lack of understanding of the complex chemical reactions and associated equilibria that occur in a working Li–S system. A new approach preparing graphene-based active cathode materials of Li-S battery with spatially confined lithium sulfides is reported. The starting graphene-embedded 2D-MoS2 was synthesized by a solvothermal method in organic solvents followed by the calcination of trapped organic solvent molecules at 800 °C to give graphene single sheets inside the 2D-MoS2 layers with 7 Å distance (MoS2-Gr-32.51). Then, it was electrochemically reduced/lithiated at potential 0.01 V vs Li+/Li generating metallic molybdenum and lithium sulfides. As a result, the structure of MoS2 multi-layers collapsed. The graphene multi-layer (ML-Graphene) was left behind and shut the lithium sulfides between the layers. The sizes of Li2Sn (n = 4–6) are bigger than the inter-layer distance of ML-Graphene, and the escape of sulfur/sulfides from the cathode into the electrolyte is physically blocked alleviating shuttle effects. The specific capacity of ML-Graphene/lithium sulfides cathode was high of 1209 mAh/gMoS2-Gr at 0.1 C (1 C = 670 mA/g). The ML-Graphene exhibited the remarkable lithium intercalation capability, and the theoretical calculation has been carried out to give 2231.4 mAh/g. Such high capacity was hybridized with the theoretical capacity of sulfur (1675 mAh/g), and the ML-Graphene composite with dichalcogenides (2D-MoS2) became a promising platform for the cathode of Li-S batteries.

Vertically Aligned 2D MoS2 Layers with Strain-Engineered Serpentine Patterns for High-Performance Stretchable Gas Sensors: Experimental and Theoretical Demonstration.

Two-dimensional (2D) molybdenum disulfide (MoS2) with vertically aligned (VA) layers exhibits significantly enriched surface-exposed edge sites with an abundance of dangling bonds owing to its intrinsic crystallographic anisotropy. Such structural variation renders the material with exceptionally high chemical reactivity and chemisorption ability, making it particularly attractive for high-performance electrochemical sensing. This superior property can be further promoted as far as it is integrated on mechanically stretchable substrates well retaining its surface-exposed defective edges, projecting opportunities for a wide range of applications utilizing its structural uniqueness and mechanical flexibility. In this work, we explored VA-2D MoS2 layers configured in laterally stretchable forms for multifunctional nitrogen dioxide (NO2) gas sensors. Large-area (>cm2) VA-2D MoS2 layers grown by a chemical vapor deposition (CVD) method were directly integrated onto a variety of flexible substrates with serpentine patterns judiciously designed to accommodate a large degree of tensile strain. These uniquely structured VA-2D MoS2 layers were demonstrated to be highly sensitive to NO2 gas of controlled concentration preserving their intrinsic structural and chemical integrity, e.g., significant current response ratios of ∼160-380% upon the introduction of NO2 at a level of 5-30 ppm. Remarkably, they exhibited such a high sensitivity even under lateral stretching up to 40% strain, significantly outperforming previously reported 2D MoS2 layer-based NO2 gas sensors of any structural forms. Underlying principles for the experimentally observed superiority were theoretically unveiled by density functional theory (DFT) calculation and finite element method (FEM) analysis. The intrinsic high sensitivity and large stretchability of VA-2D MoS2 layers confirmed in this study are believed to be applicable in sensing diverse gas species, greatly broadening their versatility in stretchable and wearable technologies.

Influence of chemical potential on shape evolution of 2D-MoS2 flakes produced by chemical vapor deposition

High-quality, ultrathin 2D-MoS2 layers with large area were grown on SiO2/Si substrates by using atmospheric pressure chemical vapor deposition (APCVD) at elevated temperatures. The growth precursors (MoO3 and S) were placed separately inside the double-zone furnace to control the growth parameters individually for better flexibility in the growth process. In this study, it was found that the shape and edge structure of the evolved MoS2 flakes were significantly influenced by the chemical potential of the Mo and S precursor concentration. In keeping with the concentration gradient of the Mo precursor (MoO3) on the substrate surface, the shape of MoS2 flakes changed from hexagonal to truncated triangle and then to triangular shapes, owing to the Mo-rich to S-rich conditions. The surface roughness and thickness of the differently shaped MoS2 flakes were studied by using atomic force microscope (AFM). Additionally, Raman and photoluminescence (PL) techniques were employed to characterize the crystalline quality, number of grown layers and optical performance of the as-grown MoS2 layers. Auger electron spectroscopy (AES) analysis and scanning electron microscopy (SEM) confirmed that the equilibrium crystal shape of the MoS2 was hexagonal under Mo-rich conditions. However, the shape of the MoS2 crystal changed to a triangle under S-rich conditions. Furthermore, the influence of chemical potential on the edge structure of the monolayer MoS2 and its effect on the equilibrium shape of the crystal were studied.

Wafer-Scale Two-Dimensional MoS2 Layers Integrated on Cellulose Substrates Toward Environmentally Friendly Transient Electronic Devices.

We explored the feasibility of wafer-scale two-dimensional (2D) molybdenum disulfide (MoS2) layers toward futuristic environmentally friendly electronics that adopt biodegradable substrates. Large-area (> a few cm2) 2D MoS2 layers grown on silicon dioxide/silicon (SiO2/Si) wafers were delaminated and integrated onto a variety of cellulose-based substrates of various components and shapes in a controlled manner; examples of the substrates include planar papers, cylindrical natural rubbers, and 2,2,6,6-tetramethylpiperidine-1-oxyl-oxidized cellulose nanofibers. The integrated 2D layers were confirmed to well preserve their intrinsic structural and chemical integrity even on such exotic substrates. Proof-of-concept devices employing large-area 2D MoS2 layers/cellulose substrates were demonstrated for a variety of applications, including photodetectors, pressure sensors, and field-effect transistors. Furthermore, we demonstrated the complete "dissolution" of the integrated 2D MoS2 layers in a buffer solution composed of baking soda and deionized water, confirming their environmentally friendly transient characteristics. Moreover, the approaches to delaminate and integrate them do not demand any chemicals except for water, and their original substrates can be recycled for subsequent growths, ensuring excellent chemical benignity and process sustainability.

Size-dependent optical properties of MoS2 nanoparticles and their photo-catalytic applications

While two-dimensional (2D) layered MoS2 nanosheets have been extensively studied owing to their fascinating optoelectronic properties, less attention has been paid to the corresponding zero-dimensional nano-crystals. In this contribution, we report the efficacy of MoS2 nanocrystals for their size tunable properties for optical and photocatalytic applications. We have synthesized differently sized (10–70 nm) crystalline, hexagonal 2H-MoS2 nanoparticles (NPs) dispersed in DMF solvent using a simple exfoliation technique. Synthesized NPs are found to exhibit size-dependent optical properties and excitation-dependent fluorescence characteristics in the visible region, which are otherwise not observed in bulk or 2D MoS2 layers. Size tunable bandgap and broad absorbance and emission spectrum covering the visible range could be exploited in the fabrication of various opto-electronic devices. Charge carrier emission dynamics of differently sized MoS2 NPs are investigated using time correlated single photon counting (TCSPC) spectroscopic technique. We found two time components, one in the order of several hundreds of ps, which arises due to the radiative recombination of charge carriers, while the other one is of the order of a few ns, which emanates from the defect states of MoS2 NPs. The average time constants are found to decrease with increase in particle size. A noticeable photocatalytic activity of the synthesized MoS2 NPs under visible light illumination for the degradation of brilliant green dye is also demonstrated for the first time and the effect of size variation of NPs in the dye degradation process is reported.

Moderate strain induced indirect bandgap and conduction electrons in MoS2 single layers

MoS2 single layers are valued for their sizeable direct bandgap at the heart of the envisaged electronic and optoelectronic applications. Here we experimentally demonstrate that moderate strain values (~2%) can already trigger an indirect bandgap transition and induce a finite charge carrier density in 2D MoS2 layers. A conclusive proof of the direct-to-indirect bandgap transition is provided by directly comparing the electronic and optical bandgaps of strained MoS2 single layers obtained from tunneling spectroscopy and photoluminescence measurements of MoS2 nanobubbles. Upon 2% biaxial tensile strain, the electronic gap becomes significantly smaller (1.45 ± 0.15 eV) than the optical direct gap (1.73 ± 0.1 eV), clearly evidencing a strain-induced direct to indirect bandgap transition. Moreover, the Fermi level can shift inside the conduction band already in moderately strained (~2%) MoS2 single layers conferring them a metallic character.

The influence of 2D MoS2 layers on the growth of GaN films by plasma-assisted molecular beam epitaxy

In the report, the growth of GaN films on the two-dimension molybdenum disulfide (2D MoS2) and c-sapphire via plasma-assisted molecular beam epitaxy (MBE) was investigated. Two kinds of MoS2 layers were prepared by pulsed laser deposition (PLD) and chemical vapor deposition (CVD) techniques. Three different surface conditions were designed for the growth of GaN films. GaN thin films in the form of polycrystalline were successfully grown on the surface of MoS2 layers. From the surface analysis, CVD technique provided an amorphous and rougher MoS2 surface for the MBE growth. On the contrary, PLD supplied a better in-plane and smoother surface for GaN growth which included more stability of surface chemical composition, higher crystallinity and better near-band-edge emission property. To compare with the growth on c-Sapphire, however, the van der Waals expitaxial growth of single-crystalline GaN films on sp2 bonded 2D MoS2 is still a challenge. The growth of GaN films on sp3 bonded c-sapphire still performed the best results in the report. In summary, we demonstrate better growth of GaN thin films on 2D MoS2 surface provided by PLD. The hetetrostructure of 3D GaN on 2D MoS2 semiconductors could be useful in the future applications of electronic and optoelectronic devices.

Improving Electrochemical Pb2+ Detection Using a Vertically Aligned 2D MoS2 Nanofilm.

Recent advancements in MoS2 nanofilms have aided in the development for important water-related environmental applications. However, a MoS2 nanofilm-coated sensor has yet to have been applied for heavy metal detection in water-related environmental samples. In this study, a novel vertically aligned two-dimensional (2D) MoS2 (edge exposed) nanofilm was applied for in situ lead ion (Pb2+) detection. The developed sensor showed an excellent linear relationship toward Pb2+ between 0 and 20 ppb at -0.45 V vs Ag/AgCl using square wave anodic stripping voltammetry (SWASV) with the improved limit of detection (LOD) of 0.3 ppb in a tap water environment. The vertically aligned 2D MoS2 sensor exhibited improved detection sensitivity (2.8 folds greater than a previous metallic [Bi] composite electrode) with lower relative standard deviation for repetitive measurements (n = 11), indicating enhanced reproducibility for Pb2+ detection. The vertically aligned 2D MoS2 layers exhibited 2.6 times higher sensitivity than horizontally aligned 2D MoS2 (basal plane exposed). Density functional theory calculations demonstrated that adsorption energy of Pb on the MoS2 side edge was much higher (4.11 eV) than those on the basal plane (0.36 and 0.07 eV). In addition, the band gap center of vertical MoS2 was found to be higher than the Pb2+ → Pb reduction potential level and capable of reducing Pb2+. Overall, the newly developed vertically aligned 2D MoS2 sensor showed excellent performance for detecting Pb2+ in a real drinking water environment with good reliability.

Experimental Realization of Few Layer Two-Dimensional MoS2 Membranes of Near Atomic Thickness for High Efficiency Water Desalination.

A globally imminent shortage of freshwater has been demanding viable strategies for improving desalination efficiencies with the adoption of cost- and energy-efficient membrane materials. The recently explored 2D transition metal dichalcogenides (2D TMDs) of near atomic thickness have been envisioned to offer notable advantages as high-efficiency membranes owing to their structural uniqueness; that is, extremely small thickness and intrinsic atomic porosity. Despite theoretically projected advantages, experimental realization of near atom-thickness 2D TMD-based membranes and their desalination efficiency assessments have remained largely unexplored mainly due to the technical difficulty associated with their seamless large-scale integration. Herein, we report the experimental demonstration of high-efficiency water desalination membranes based on few-layer 2D molybdenum disulfide (MoS2) of only ∼7 nm thickness. Chemical vapor deposition (CVD)-grown centimeter-scale 2D MoS2 layers were integrated onto porous polymeric supports with well-preserved structural integrity enabled by a water-assisted 2D layer transfer method. These 2D MoS2 membranes of near atomic thickness exhibit an excellent combination of high water permeability (>322 L m-2 h-1 bar-1) and high ionic sieving capability (>99%) for various seawater salts including Na+, K+, Ca2+, and Mg2+ with a range of concentrations. Moreover, they present near 100% salt ion rejection rates for actual seawater obtained from the Atlantic coast, significantly outperforming the previously developed 2D MoS2 layer membranes of micrometer thickness as well as conventional reverse osmosis (RO) membranes. Underlying principles behind such remarkably excellent desalination performances are attributed to the intrinsic atomic vacancies inherent to the CVD-grown 2D MoS2 layers as verified by aberration-corrected electron microscopy characterization.

Inorganic\u2013organic nanohybrid of MoS2-PANI for advanced photocatalytic application

In this work, the fabrication of MoS2-Polyaniline (PANI) nanocomposites, by in situ polymerization, has been described and its application as a photocatalyst for the degradation of organic pollutants such as methylene blue (MB) and 4-chlorophenol (4-CP), has been reported. The disadvantages of MoS2 such as poor electronic conductivity and agglomeration between the nanosheets, was overcome by intercalating 2D MoS2 layers with 1D conducting polymer, Polyaniline (PANI). The composite material was characterised by SEM, TEM, BET, XRD, FTIR, UV–Vis spectroscopy and XPS, indicating proper intercalation between MoS2 nanosheets and PANI. Consequently, the synthesized composites were used for the degradation of MB and 4-CP, followed by kinetic investigations to determine the rate kinetics. The photoactivity of the nanocomposite is explained by the transfer of photogenerated electrons from PANI to the CB of MoS2, thus preventing the direct recombination of electrons and holes. Hence, a positive synergistic effect between MoS2 and PANI resulted in efficient photocatalytic degradation of organic dyes like MB.

Recent advances in molybdenum disulfide-based electrode materials for electroanalytical applications.

The primary objective of this review article is to summarize the development and structural diversity of 2D/3D molybdenum disulfide (MoS2) based modified electrodes for electrochemical sensors and biosensor applications. Hydrothermal, mechanical, and ultrasonic techniques and solution-based exfoliation have been used to synthesize graphene-like 2D MoS2 layers. The unique physicochemical properties of MoS2 and its nanocomposites, including high mechanical strength, high carrier transport, large surface area, excellent electrical conductivity, and rapid electron transport rate, render them useful as efficient transducers in various electrochemical applications. The present review summarizes 2D/3D MoS2-based nanomaterials as an electrochemical platform for the detection and analysis of various biomolecules (e.g., neurotransmitters, NADH, glucose, antibiotics, DNA, proteins, and bacteria) and hazardous chemicals (e.g., heavy metal ions, organic compounds, and pesticides). The substantial improvements that have been achieved in the performance of enzyme-based amperometry, chemiluminescence, and nucleic acid sensors incorporating MoS2-based chemically modified electrodes are also addressed. We also summarize key sensor parameters such as limits of detection (LODs), sensitivity, selectivity, response time, and durability, as well as real applications of the sensing systems in the environmental, pharmaceutical, chemical, industrial, and food analysis fields. Finally, the remaining challenges in designing MoS2 nanostructures suitable for electroanalytical applications are outlined. Graphical abstract • MoS2 based materials exhibit high conductivity and improved electrochemical performance with great potential as a sensing electrode. • The role of MoS2 nanocomposite films and their detection strategies were reviewed. • Biomarkers detection for disease identification and respective clinical treatments were discussed. • Future Challenges, as well as possible research development for "MoS2 nanocomposites", are suggested.

An in-situ growth approach to 2D MoS2-2D PbS heterojunction composites with improved photocatalytic activity

The advantage of 2D-2D heterojunction over 2D-0D and 2D-1D heterojunction is that it has larger interface area, which results in the shorter migration distance of photo-induced charge carriers, and can therefore separate the electron-hole pairs more effectively. In this work, to form 2D-2D heterojunction, PbS nanosheets were grown in situ on 2D MoS2 layers via. solvothermal process. The formation of 2D MoS2-2D PbS composites has been confirmed by XRD, Raman, TEM, and EDS analysis. The area of PbS nanosheets attached on MoS2 can be controlled by changing the concentration of PbS precursor in reaction solution. Compared with pristine MoS2, MoS2-PbS composites showed improved light absorption property and enhanced photocatalytic ability using methylene blue as the target of degradation. The optimized composite displayed a photocurrent 5 times higher than that of pristine MoS2.

Centimeter-Scale Periodically Corrugated Few-Layer 2D MoS2 with Tensile Stretch-Driven Tunable Multifunctionalities.

Two-dimensional (2D) transition metal dichalcogenide (TMD) layers exhibit superior optical, electrical, and structural properties unattainable in any traditional materials. Many of these properties are known to be controllable via external mechanical inputs, benefiting from their extremely small thickness coupled with large in-plane strain limits. However, realization of such mechanically driven tunability often demands highly complicated engineering of 2D TMD layer structures, which is difficult to achieve on a large wafer scale in a controlled manner. Herein, we explore centimeter-scale periodically corrugated 2D TMDs, particularly 2D molybdenum disulfide (MoS2), and report their mechanically tunable multifunctionalities. We developed a water-assisted process to homogeneously integrate few layers of 2D MoS2 on three-dimensionally corrugated elastomeric substrates on a large area (>2 cm2). The evolution of electrical, optical, and structural properties in these three-dimensionally corrugated 2D MoS2 layers was systematically studied under controlled tensile stretch. We identified that they present excellent electrical conductivity and photoresponsiveness as well as systematically tunable surface wettability and optical absorbance even under significant mechanical deformation. These novel three-dimensionally structured 2D materials are believed to offer exciting opportunities for large-scale, mechanically deformable devices of various form factors and unprecedented multifunctionalities.

Three dimensionally-ordered 2D MoS2 vertical layers integrated on flexible substrates with stretch-tunable functionality and improved sensing capability.

The intrinsically anisotropic crystallinity of two-dimensional (2D) transition metal dichalcogenide (2D TMD) layers enables a variety of intriguing material properties which strongly depend on the physical orientation of constituent 2D layers. For instance, 2D TMDs with vertically-aligned layers exhibit numerous dangling bonds on their 2D layer edge sites predominantly exposed on the surface, projecting significantly improved physical and/or chemical adsorption capability compared to their horizontally-oriented 2D layer counterparts. Such property advantages can be further promoted as far as the material can be integrated onto unconventional substrates of tailored geometry/functionality, offering vast opportunities for a wide range of applications which demand enhanced surface area/reactivity and mechanical flexibility. Herein, we report a new form of 2D TMDs, i.e., three-dimensionally ordered 2D molybdenum disulfide (2D MoS2) with vertically-aligned layers integrated on elastomeric substrates and explore their tunable multi-functionalities and technological promise. We grew large-scale (>2 cm2) vertically-aligned 2D MoS2 layers using a three-dimensionally patterned silicon dioxide (SiO2) template and directly transferred/integrated them onto flexible polydimethylsiloxane (PDMS) substrates by taking advantage of the distinguishable water-wettability of 2D MoS2vs. SiO2. The excellent structural integrity of the integrated vertical 2D MoS2 layers was confirmed by extensive spectroscopy/microscopy characterization. In addition, the stretch-driven unique tunability of their optical and surface properties was also examined. Moreover, we applied this material for flexible humidity sensing and identified significantly improved (>10 times) sensitivity over conventionally-designed horizontal 2D MoS2 layers, further confirming their high potential for unconventional flexible technologies.

Enhanced sulfurization reaction of molybdenum using a thermal cracker for forming two-dimensional MoS2 layers.

We propose a method to fabricate two-dimensional (2D) molybdenum disulfide (MoS2) layers to overcome issues in typical fabrication processes by promoting the sulfurization reaction of molybdenum (Mo). A thin sputtered-Mo layer was sulfurized using a sulfur (S) thermal cracker to form 2D MoS2 layers. The effects of key process parameters such as cracking-zone temperature (TC-zone), thickness of the sputtered-Mo layer, and Ar pressure during deposition of the Mo layer were systematically investigated. The degree of thermal treatment of evaporated S vapor is controlled by varying TC-zone. The higher TC-zone enabled easy formation of thin MoS2 layers at a low substrate temperature of 250 °C due to the greatly enhanced sulfurization reaction. The thickness of the final MoS2 layers was controlled by changing the initial thickness of the sputtered-Mo film. Ultra-thin MoS2 film about 2-layers-thick was obtained by sulfurizing a 2 Å-thick Mo film. The chemical state of the MoS2 layers largely depended on the Ar pressure during the sputtering process of the initial Mo. Lower Ar pressure enhanced MoS2 formation due to more efficient substitution of the MoS2 phase for the MoO3 phase. By using the S thermal cracker, we demonstrate a method to easily fabricate 2D MoS2 layers, excluding some problematic issues such as toxic and expensive reactants, non-vacuum conditions susceptible to contamination, and high substrate temperature.

A Raman metrology approach to quality control of 2D MoS2 film fabrication

Promising electronic and optoelectronic properties of two-dimensional (2D) materials have spurred research into large area fabrication through vapour deposition and etching. However, robust and efficient non destructive characterization techniques are required in order to reliably produce good quality uniform layers. Here, we present a Raman spectroscopy approach for characterization of the quality and a systematic study of the impact of process parameters for the production of 2D MoS2 layers. We also present the application of this characterization technique for controlled layer by layer etching of multilayer MoS2.

Multiflake Thin Film Electronic Devices of Solution Processed 2D MoS2 Enabled by Sonopolymer Assisted Exfoliation and Surface Modification

The solvent-assisted exfoliation of transition metal dichalchogenides (TMDs) is a promising method for preparing scalable quantities of two-dimensional nanomaterials dispersed in a liquid phase. However, low concentrations and the restacking/aggregation of TMD layers remain challenges to the solution based preparation of large-area electronic devices. Here we present advances in the exfoliation and solution processing of 2D MoS2 that are subsequently leveraged to prepare and electronically probe homogeneous multiflake thin-film devices. We report that sonopolymer, formed when using 1,2-dichlorobenzene (DCB) as a solvent, plays a critical role in affording stable dispersions (up to 0.5 mg mL–1) of few-layer MoS2 flakes in the 2H phase after only 6 h of low-power sonication. After removing the sonopolymer using a washing procedure, alkyl-trichlorosilane surfactants were used to prevent the restacking of 2D MoS2 layers and create stable dispersions with concentrations as high as 85 mg mL–1. In spin-coated multiflake thin films as thin as 20 nm, electron transport parallel to the substrate was quantifiable over channel lengths of 50 μm owing to the homogeneous film formation. By further varying the alkyl-trichlorosilane chain length we show that a trade-off between dispersibility (film homogeneity) and electronic insulation from the surfactant leads to a maximum (multiflake) electron mobility of 0.02 cm2 V–1 s–1 using hexyl-trichlorosilane modified MoS2 in the direction perpendicular to the substrate as measured by space-charge limited current devices.

Synthesis of MoS2 nano-petal forest supported on carbon nanotubes for enhanced field emission performance

We report the fabrication of a three-dimensional forest of highly crystalline two-dimensional (2D) molybdenum disulfide (MoS2) nano-petals encapsulating vertically aligned carbon nanotubes (CNT) in a core-shell configuration. Growth was conducted via magnetron sputtering at room temperature and it was found that the nano-petal morphology was formed only when a critical threshold in sputter deposition time was reached. Below this threshold, an amorphous tubular structure composed of mainly molybdenum oxides dominates instead. The presence of the MoS2 nano-petals was shown to impart photoluminescence to the CNTs, in addition to significantly enhancing their electron emission properties, where the turn-on field was lowered from 2.50 Vμm−1 for pristine CNTs to 0.80 Vμm−1 for MoS2-CNT heterostructures fabricated at 30 min sputter deposition time. Photoluminescence was detected at wavelengths of approximately 684 nm and 615 nm, with the band at 684 nm gradually blue-shifting as sputter time was increased. These results demonstrate that it is possible to synthesize 2D MoS2 layers without the need for chemical routes and high growth temperatures.