MoS2 Single Crystals Research Articles

Gate-Controlled Potassium Intercalation and Superconductivity in Molybdenum Disulfide.

Intercalation of guest ions into a van der Waals (vdW) gap in layered materials is a powerful route to create novel material phases and functionalities. Ionic gating is a technique to control the motions and configuration of ions for both intercalation and surface electrostatic doping. The advance of ionic gating enables the in situ probe of dynamics of ion diffusion, carrier doping, and transport properties. Here we performed in situ resistivity and Raman experiments on the potassium ion (K+) intercalation of single-crystal MoS2 and constructed a temperature-carrier density phase diagram. The K+-intercalation induces a structural transition from the prismatically coordinated phase to the octahedrally coordinated phase, where anisotropic three-dimensional superconductivity and a possible charge density wave state were observed. The present ionic gating offers a comprehensive view of the intercalated phases and proves that the electrostatically induced superconductivity is distinct from that in the intercalated phase.

Layer Number and Stacking Engineering of MoS2 Crystals for High-Performance Polarization-Sensitive Photodetector.

The layer and stacking engineering of two-dimensional (2D) transition-metal dichalcogenides (TMDs) gives rise to novel phenomena and multiapplications; thus, TMDs have garnered considerable attention. However, the precisely customized fabrication of stacked 2D materials to date is largely limited to the lack of effective and controllable growth strategies, prone to the unpredictable stacking orders and randomly distributed nucleation sites. Here, we devise an optimized chemical vapor deposition approach for modulating the MoS2 single crystals from monolayer to multilayer with diverse stacking configurations. Significantly, the phototransistor based on monolayer MoS2 single crystal exhibits an ultrasensitive performance with a high photoresponsivity (R) of 3.3 × 104 A W-1 and a remarkable detectivity (D*) of above 1.7 × 1014 Jones at 405 nm light illumination. Ultralow-frequency and angle-resolved polarized Raman spectroscopy is used to systematically uncover the delicate interlayer interactions and crystallographic anisotropy. Moreover, the polarization-sensitive photodetectors using 1-3L MoS2 show a layer number-dependent anisotropic performance, with dichroism ratios of 1.36, 1.44, and 1.52. This work offers a promising method to not only enable the fabrication of new customized layer-, stacking-, and twist-2D materials but also provides the foundation for the development of advanced polarization-sensitive and optoelectronic devices based on stacking transitions.

Strongly Enhanced Electronic Bandstructure Renormalization by Light in Nanoscale Strained Regions of Monolayer MoS2/Au(111) Heterostructures.

Understanding and controlling the photoexcited quasiparticle (QP) dynamics in monolayer (ML) transition metal dichalcogenides (TMDs) lays the foundation for exploring the strongly interacting, nonequilibrium two-dimensional (2D) QP and polaritonic states in these quantum materials and for harnessing the properties emerging from these states for optoelectronic applications. In this study, scanning tunneling microscopy/spectroscopy (STM/scanning tunneling spectroscopy) with light illumination at the tunneling junction is performed to investigate the QP dynamics in ML MoS2 on an Au(111) substrate with nanoscale corrugations. The corrugations on the surface of the substrate induce nanoscale local strain in the overlaying ML MoS2 single crystal, which result in energetically favorable spatial regions where photoexcited QPs, including excitons, trions, and electron-hole plasmas, accumulate. These strained regions exhibit pronounced electronic bandstructure renormalization as a function of the photoexcitation wavelength and intensity as well as the strain gradient, implying strong interplay among nanoscale structures, strain, and photoexcited QPs. In conjunction with the experimental work, we construct a theoretical framework that integrates nonuniform nanoscale strain into the electronic bandstructure of a ML MoS2 lattice using a tight-binding approach combined with first-principle calculations. This methodology enables better understanding of the experimental observation of photoexcited QP localization in the nanoscale strain-modulated electronic bandstructure landscape. Our findings illustrate the feasibility of utilizing nanoscale architectures and optical excitations to manipulate the local electronic bandstructure of ML TMDs and to enhance the many-body interactions of excitons, which is promising for the development of nanoscale energy-adjustable optoelectronic and photonic technologies, including quantum emitters and solid-state quantum simulators for interacting exciton polaritons based on engineered periodic nanoscale trapping potentials.

Mechanisms of Controllable Growth and Ohmic Contact of Two-Dimensional Molybdenum Disulfide: Insight from Atomistic Simulations.

ConspectusTwo-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), in particular molybdenum disulfide (MoS2), have recently attracted huge interest due to their proper bandgap, high mobility at 2D limit, and easy-to-integrate planar structure, which are very promising for extending Moore's law in postsilicon electronics technology. Great effort has been devoted toward such a goal since the demonstration of protype MoS2 devices with high room-temperature on/off current ratios, ultralow standby power consumption, and atomic level scaling capacity down to sub-1-nm technology node. However, there are still several key challenges that need to be addressed prior to the real application of MoS2-based electronics technology. The controllable growth of wafer-scale single-crystal MoS2 on industry-compatible insulating substrates is the prerequisite of application while the currently synthesized MoS2 films mostly are polycrystalline with limited sizes of single-crystal domains and may involve metal substrates. The precise layer-control is also very important for MoS2 growth since its electronic properties are layer-dependent, whereas the layer-by-layer growth of multilayer MoS2 dominated by the van der Waals (vdW) epitaxy leads to poor thickness uniformity and noncontinuously distributed domains. High density up to 1013 cm-2 of sulfur vacancies (SVs) in grown MoS2 can cause unfavorable carrier scatting and electronic properties variations and will inevitably disturb the device performance. The dangling-bond-free surface of MoS2 gives rise to an inherent vdW gap at metal-semiconductor (M-S) contact, which leads to high electrical resistance and poor current-delivery capability at the contact interface and thereby substantially limits the performances of MoS2 devices.In this Account, we briefly review recent experimental and theoretical attempts for addressing the aforementioned challenges and present our own insights from atomistic simulations. We theoretically revealed the vital role of substrate steps for guiding unidirectional nucleation of monolayer MoS2 and uniform nucleation and edge-aligned growth of bilayer MoS2 by advanced simulations. The established thermodynamic mechanisms have successfully directed the experimental works on the controllable growth of 2 in. single-crystal monolayer and centimeter-scale uniform bilayer MoS2. The postgrowth repair mechanism of SV defect in MoS2 via thiol chemistry treatment has been theoretically explored with the consideration of side reaction of surface functionalization to help experimentally reduce SV defect density by 75%. Beyond the atomic level understanding, theoretical simulations proposed the electronic states hybridization mechanism across the semimetal-MoS2 vdW interface, thereby guiding experimental effort for realizing Ohmic contact at the MoS2-Sb(0112) vdW interface with record-low contact resistance.These advances provide a sound basis with an atomic-level understanding for addressing the related issues. However, there are still notable gaps in terms of system size and time scale of dynamics between atomistic simulations and experimental observations for the studies of MoS2 growth and interfaces. The combination of multiscale simulations and artificial intelligence technology is expected to narrow these gaps and provide a more insightful understanding of the controllable growth and interfacial properties modulation of MoS2. We conclude the Account with the standing challenges and outlook on future research directions from the theoretical perspective.

Comparative study of sodium and potassium compounds as promoters for growth of monolayer MoS2 with high crystal quality on SiO2/Si substrate

Monolayer MoS2 is promising candidate for fabrication of optoelectronic devices due to its direct bandgap nature and high carrier mobility. Alkali metal compounds have been demonstrated to be helpful promoters for the growth of large single crystal monolayer MoS2 on SiO2/Si substrate. However, the catalytic mechanism of alkali metal compounds is still under debate. Herein, we compared the surface morphology, optical properties, and electrical properties of monolayer MoS2 flakes grown on SiO2/Si substrate assisted by promoters containing potassium or sodium cations and halogen (chlorine) or non-halogen (hydroxide) anions, i.e. NaCl, NaOH, KCl and KOH. Based on the analysis of existing growth mechanism, we proposed that the alkali metal cation, plays a dominant role in promoting the lateral growth of monolayer MoS2 and obtaining high crystal quality. Furthermore, potassium has a greater promoting effect than sodium. By optimizing growth conditions, monolayer triangular MoS2 flakes with large lateral size over 160 μm were grown assisted by KCl promoter. Raman and PL spectra verified excellent crystal quality of the flakes, with typical electron mobilities of 2.98 and 20 cm2 V−1 s−1 for the back-gated filed effect transistors fabricated on as-grown and fresh SiO2/Si substrates, respectively.

The nucleation mechanism of MoS2 on Au(111) surface

Controllable preparation of two-dimensional MoS2 single crystal thin films is the key to its development and application. Chemical vapor deposition (CVD) is considered one of the most promising methods for large-scale production of 2D MoS2 films. However, at present, the single crystal MoS2 films prepared by CVD have defects and insufficient sizes. The reason may be that the CVD growth mechanism of MoS2 is still unclear. In this paper, density functional theory (DFT) and molecular dynamics (MD) simulations are used to systematically explore the nucleation mechanism of MoS2 grown on Au (111) surface with molybdenum powder and H2S as precursors. In our theoretical study, some key links of MoS2 nucleation have been clearly displayed, such as deposition of molybdenum, dehydrogenation of H2S, lifting of Mo atoms and so on. This study provides a deep understanding of the nucleation of MoS2 during CVD growth and theoretical basis for the synthesis of various TMDs.

Nanoscale Adhesion and Material Transfer at 2D MoS2-MoS2 Interfaces Elucidated by In Situ Transmission Electron Microscopy and Atomistic Simulations.

Low-dimensional materials, such as MoS2, hold promise for use in a host of emerging applications, including flexible, wearable sensors due to their unique electrical, thermal, optical, mechanical, and tribological properties. The implementation of such devices requires an understanding of adhesive phenomena at the interfaces between these materials. Here, we describe combined nanoscale in situ transmission electron microscopy (TEM)/atomic force microscopy (AFM) experiments and simulations measuring the work of adhesion (Wadh) between self-mated contacts of ultrathin nominally amorphous and nanocrystalline MoS2 films deposited on Si scanning probe tips. A customized TEM/AFM nanoindenter permitted high-resolution imaging and force measurements in situ. The Wadh values for nanocrystalline and nominally amorphous MoS2 were 604 ± 323 mJ/m2 and 932 ± 647 mJ/m2, respectively, significantly higher than previously reported values for mechanically exfoliated MoS2 single crystals. Closely matched molecular dynamics (MD) simulations show that these high values can be explained by bonding between the opposing surfaces at defects such as grain boundaries. Simulations show that as grain size decreases, the number of bonds formed, the Wadh and its variability all increase, further supporting that interfacial covalent bond formation causes high adhesion. In some cases, sliding between delaminated MoS2 flakes during separation is observed, which further increases the Wadh and the range of adhesive interaction. These results indicate that for low adhesion, the MoS2 grains should be large relative to the contact area to limit the opportunity for bonding, whereas small grains may be beneficial, where high adhesion is needed to prevent device delamination in flexible systems.

Epitaxy of wafer-scale single-crystal MoS2 monolayer via buffer layer control

Monolayer molybdenum disulfide (MoS2), an emergent two-dimensional (2D) semiconductor, holds great promise for transcending the fundamental limits of silicon electronics and continue the downscaling of field-effect transistors. To realize its full potential and high-end applications, controlled synthesis of wafer-scale monolayer MoS2 single crystals on general commercial substrates is highly desired yet challenging. Here, we demonstrate the successful epitaxial growth of 2-inch single-crystal MoS2 monolayers on industry-compatible substrates of c-plane sapphire by engineering the formation of a specific interfacial reconstructed layer through the S/MoO3 precursor ratio control. The unidirectional alignment and seamless stitching of MoS2 domains across the entire wafer are demonstrated through cross-dimensional characterizations ranging from atomic- to centimeter-scale. The epitaxial monolayer MoS2 single crystal shows good wafer-scale uniformity and state-of-the-art quality, as evidenced from the ~100% phonon circular dichroism, exciton valley polarization of ~70%, room-temperature mobility of ~140 cm2v−1s−1, and on/off ratio of ~109. Our work provides a simple strategy to produce wafer-scale single-crystal 2D semiconductors on commercial insulator substrates, paving the way towards the further extension of Moore’s law and industrial applications of 2D electronic circuits.

Synthesis of two-dimensional MoO2 nanoplatelets and its multistep sulfurization into MoS2

To control the growth of layered two-dimensional structures, such as transition metal dichalcogenide materials or heterostructures, understanding the growth mechanism is crucial. Here, we report the synthesis of ultra-thin MoO2 nanoplatelets through the sublimation of MoO3. Rhombus MoO2 nanoplatelets with the P21/c space group were characterized using various microscopic and spectroscopic techniques. Introducing sulfur sources into the chemical vapor deposition system also leads to the formation of monoclinic MoO2 nanoflakes due to the incomplete sulfurization of MoO3. With a gradual increase in the vapor concentration of sulfur, MoO3 undergoes stepwise reduction into MoS2/MoO2 and eventually into MoS2. Additionally, utilizing MoO2 as a precursor for Mo sources enables the formation of monolayer MoS2 single crystals. This work provides an effective approach for growing MoO2 nanoplatelets and elucidates the mechanism behind the stepwise sulfurization of MoO3.

Controlled Sixfold Symmetric Exfoliation of Oriented MoS2 Monolayers by Coulomb Force

AbstractAtoms, molecules, and nanoparticles can be spatially manipulated by an atomic force microscopy (AFM) tip, through van der Waals (vdW) and/or Coulomb forces. These point‐to‐point manipulations are highly accurate at nanoscale, facilitating the construction and modification of nanostructures. Nevertheless, it is difficult to manipulate 2D layers in vdW crystals by an AFM tip, because the tip‐induced attractive force is usually insufficient to outcompete the interlaminar vdW forces. Herein, manipulation of the surface layers on a MoS2 single crystal by a conductive AFM tip is successfully reported. By applying a bias between the tip and MoS2, the Coulomb attractive force allows the topmost MoS2 layers to be picked up. These exfoliated layers are deformed into micron‐sized bubbles with sixfold symmetry, which are composed of high‐quality monolayers and visually reflecting the hexagonal lattice orientation. The underlying mechanisms of the sixfold symmetric exfoliation and the formation of monolayers are discussed by in situ monitoring of the tunneling volt‐ampere characteristics and simulation of the force distribution. The findings open a new route to obtain high‐quality transition metal dichalcogenide (TMD) monolayers and their derived nanostructures on the surface of TMD single crystals for optoelectronic and photonic device applications.

Enhanced Photogating Gain in Scalable MoS2 Plasmonic Photodetectors via Resonant Plasmonic Metasurfaces.

Absorption of photons in atomically thin materials has become a challenge in the realization of ultrathin, high-performance optoelectronics. While numerous schemes have been used to enhance absorption in 2D semiconductors, such enhanced device performance in scalable monolayer photodetectors remains unattained. Here, we demonstrate wafer-scale integration of monolayer single-crystal MoS2 photodetectors with a nitride-based resonant plasmonic metasurface to achieve a high detectivity of 2.58 × 1012 Jones with a record-low dark current of 8 pA and long-term stability over 40 days. Upon comparison with control devices, we observe an overall enhancement factor of >100; this can be attributed to the local strong EM field enhanced photogating effect by the resonant plasmonic metasurface. Considering the compatibility of 2D semiconductors and hafnium nitride with the Si CMOS process and their scalability across wafer sizes, our results facilitate the smooth incorporation of 2D semiconductor-based photodetectors into the fields of imaging, sensing, and optical communication applications.

Converting the Bulk Transition Metal Dichalcogenides Crystal into Stacked Monolayers via Ethylenediamine Intercalation.

We report the synthesis of ethylenediamine-intercalated NbSe2 and Li-ethylenediamine-intercalated MoSe2 single crystals with increased interlayer distances and their electronic structures measured by means of angle-resolved photoemission spectroscopy (ARPES). X-ray diffraction patterns and transmission electron microscopy images confirm the successful intercalation and an increase in the interlayer distance. ARPES measurement reveals that intercalated NbSe2 shows an electronic structure almost identical to that of monolayer NbSe2. Intercalated MoSe2 also returns the characteristic feature of the monolayer electronic structure, a direct band gap, which generates sizable photoluminescence even in the bulk form. Our results demonstrate that the properties and phenomena of the monolayer transition metal dichalcogenides can be achieved with large-scale bulk samples by blocking the interlayer interaction through intercalation.

The effect of Ar plasma on the space-confined growth of MoS2 with low-pressure chemical vapor deposition

Plasma assisted low-pressure chemical vapor deposition has previously been shown to allow for large area growth of a variety of 2D materials, such as graphene and boron nitride. However, it also presented with degradation of electronic properties owing to decreases in grain sizes and increased inclusion of defects. In this work, we report on the influence of an Ar plasma during the growth of MoS2. We produce hexagonal and triangular single crystal 2D MoS2 with sizes up to 10 µm, similar to that achieved without plasma present. Raman analysis also exhibits no significant changes with plasma. However, the plasma does induce changes to the morphology of the MoS2 crystals, leading to non-uniform edge structures with the degree of non-uniformity scaling with plasma power. Comparing the overall morphology at different temperatures and amounts of precursor material suggests that plasma increases the availability of Mo for growth, which is further evidenced by increased growth zones. Therefore, the use of an Ar plasma may provide a means to reduce required precursor quantities without significantly compromising the overall structure of the resulting MoS2 crystals.

Modulation Effect of Substrate Interactions on Nucleation and Growth of MoS2 on Silica

Chemical vapor deposition is a well-established bottom-up technique to produce a high-quality single-crystal MoS2 film. In this technique, the substrate (e.g., silica) plays a crucial role in the segregation and chemical interaction of precursors to form grain-sized MoS2. However, the mechanisms of the surface interactions that influence the properties of MoS2 during growth are still poorly understood. Here, we combine ReaxFF reactive molecular dynamics simulations, density functional theory (DFT) calculations, and experimental growth of MoS2 to provide an atomic insight into the coupling between the surface chemistry and the MoS2 nucleation and growth on a silica surface. Our experimental results show that the dehydroxylated surface stays mainly inert during the MoO3 flow, while the presence of hydroxyl groups leads to MoO3 nucleation on the substrate. ReaxFF and DFT simulations further confirm that the reaction between MoO3 and the hydroxylated surface is both thermodynamically and kinetically driven, indicating that hydroxyl groups formed on silica enhance the chemical reactivity of the surface toward MoO3 molecules and promote the growth. Additionally, the MoS2 growth on the hydroxylated silica support initiates with MoO3 nucleation followed by the chalcogen–surface interactions. Moreover, the existence of the substrate catalyzes the growth by lowering the growth temperature, providing an effective way for energy saving and cost reduction. These results demonstrate the intricate role of surface engineering in controlling and promoting large-area MoS2 growth.

Highly Reproducible Epitaxial Growth of Wafer-Scale Single-Crystal Monolayer MoS2 on Sapphire.

2D semiconducting transition-metal dichalcogenides (TMDs) have attracted considerable attention as channel materials for next-generation transistors. To meet the industry needs, large-scale production of single-crystal monolayer TMDs in highly reproducible and energy-efficient manner is critically significant. Herein, it is reported that the high-reproducible, high-efficient epitaxial growth of wafer-scale monolayer MoS2 single crystals on the industry-compatible sapphire substrates, by virtue of a deliberately designed "face-to-face" metal-foil-based precursor supply route, carbon-cloth-filter based precursor concentration decay strategy, and the precise optimization of the chalcogenides and metal precursor ratio (i.e., S/Mo ratio). This unique growth design can concurrently guarantee the uniform release, short-distance transport, and moderate deposition of metal precursor on a wafer-scale substrate, affording high-efficient and high-reproducible growth of wafer-scale single crystals (over twoinches, six times faster than usual). Moreover, the S/Mo precursor ratio is found as a key factor for the epitaxial growth of MoS2 single crystals with rather high crystal quality, as convinced by the relatively high electronic performances of related devices. This work demonstrates a reliable route for the batch production of wafer-scale single-crystal 2D materials, thus propelling their practical applications in highly integrated high-performance nanoelectronics and optoelectronics.

Vapor-Liquid-Solid Growth of Site-Controlled Monolayer MoS2 Films Via Pressure-Induc ed Supercritical Phase Nucleation.

In this study, a novel pressure-induced supercritical phase nucleation method is proposed to synthesize monolayer MoS2 films, which is promoter free and can avoid contamination of films derived from these heterogeneous promoters in most of the existing techniques. The low-crystallinity and size-controlled MoO2(acac)2 particles are recrystallized on the substrate via the pressure-sensitive solvent capacity of supercritical CO2 and these particles are used as growth sites. The size of single-crystal MoS2 on the substrate is found to be dependent on the wetting area of the pyrolyzed precursor droplets (MoO2) on the surface, and the formation of continuous films with high coverage is mainly controlled by the coalescence of MoO2 droplets. It is enhanced by the increase of the nucleation site density, which can be adjusted by the supersaturation of the supercritical fluid solution. Our findings pave a new way for the controllable growth of MoS2 and other two-dimensional materials and provide sufficient and valuable evidence for vapor-liquid-solid growth.

Direct CVD Synthesis of MoS2 Monolayers on Glass by Carbothermal Reduction

Chemical vapor deposition (CVD) synthesis for two-dimensional (2D) transition-metal dichalcogenides (TMDCs) is fundamentally important for realizing high-quality single crystals of TMDCs for future electronic and optoelectronic device applications. However, CVD synthesis of TMDCs generally requires a high synthetic temperature (>700 °C), which limits the choice of growth substrates and their broad applications. In this work, we present direct CVD synthesis of 2D MoS2 on glass. The CVD growth temperature was significantly decreased to 500 °C by employing carbothermal reduction, which uses carbon as the catalyst for reducing the thermal decomposition temperature of MoO3 precursors. MoS2 single crystals grown on glass showed no observable degradation in electrical, optical, and structural properties compared to MoS2 grown at high temperatures. The MoS2 grown on glass exhibited field effect mobility around 7.6 cm2 V–1 s–1 and a high ON/OFF ratio of up to 107, photoresponsivity up to 40 A/W, and stable and repeatable photocurrent. These findings demonstrate a promising strategy in the CVD growth of 2D materials and the design of their flexible and transparent devices.

Origin of electrically induced defects in monolayer MoS2 grown by chemical vapor deposition

Defects in MoS2 play substantial role in determining the performance of MoS2-based field-effect transistors. Typically, growth/synthesis process conditions determine the type and concentration of defects. Here, we show that defects are also introduced by prolonged operation of single crystal chemical vapor deposition-grown monolayer MoS2 transistors which hinder the overall performance. Depending on the electrical stress conditions, these defects result in threshold voltage instabilities, enhanced channel conductance, improved screening of charged impurity scattering sites and possibly better thermal management in MoS2 transistors. It turns out that a piezoelectric response in MoS2 leads to permanent change in the material’s molecular configuration thereby causing other effects like suppressed hopping transport within the channel, increased free electron concentration, prominent metal-insulator transition and reduction in channel potential with or without increasing sulfur vacancy concentration. As these defects are progressively introduced in the channel, the thermal dissipation capability of our MoS2 transistors improved due to enhanced channel-dielectric coupling. Such variations in the device performance due to spontaneous response to high electric field trigger a need to reconsider supply voltage requirements of MoS2-based electronic circuits for low-power logic applications.

Chiral molecule induced valley polarization enhancement of MoS2.

Monolayers of transition metal dichalcogenides (TMDCs) are atomically thin direct-bandgap semiconductors with potential applications in nanoelectronics, opto-electronics, and electrochemical sensing. Recent theoretical and experimental results have suggested that they are ideal systems for exploiting the valley degrees of freedom of Bloch electrons. Here, we report detailed studies of the opto-valleytronic properties of a chiral histidine molecule embedded in monolayer MoS2 single crystals grown via chemical vapor deposition. By irradiating MoS2 with circularly polarized light and measuring the resulting spatially resolved circularly polarized emission, we find the existence of a significantly increased circular polarization for D-histidine doped MoS2. The increased valley contrast is attributed to the selective enhancement of both the excitation and emission rates having one particular handedness of the circular polarization. These results provide a promising pathway to enhance the valley contrast for monolayer TMDCs at room temperature.

High-throughput dry transfer and excitonic properties of twisted bilayers based on CVD-grown transition metal dichalcogenides.

van der Waals (vdW) layered materials have attracted much attention because their physical properties can be controlled by varying the twist angle and layer composition. However, such twisted vdW assemblies are often prepared using mechanically exfoliated monolayer flakes with unintended shapes through a time-consuming search for such materials. Here, we report the rapid and dry fabrication of twisted multilayers using chemical vapor deposition (CVD) grown transition metal chalcogenide (TMDC) monolayers. By improving the adhesion of an acrylic resin stamp to the monolayers, the single crystals of various TMDC monolayers with desired grain size and density on a SiO2/Si substrate can be efficiently picked up. The present dry transfer process demonstrates the one-step fabrication of more than 100 twisted bilayers and the sequential stacking of a twisted 10-layer MoS2 single crystal. Furthermore, we also fabricated hBN-encapsulated TMDC monolayers and various twisted bilayers including MoSe2/MoS2, MoSe2/WSe2, and MoSe2/WS2. The interlayer interaction and quality of dry-transferred, CVD-grown TMDCs were characterized by using photoluminescence (PL), cathodoluminescence (CL) spectroscopy, and cross-sectional electron microscopy. The prominent PL peaks of interlayer excitons can be observed for MoSe2/MoS2 and MoSe2/WSe2 with small twist angles at room temperature. We also found that the optical spectra were locally modulated due to nanosized bubbles, which are formed by the presence of interface carbon impurities. The present findings indicate the widely applicable potential of the present method and enable an efficient search of the emergent optical and electrical properties of TMDC-based vdW heterostructures.