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1.
2D atomic sheets of transition metal dichalcogenides (TMDs) have a tremendous potential for next‐generation optoelectronics since they can be stacked layer‐by‐layer to form van der Waals (vdW) heterostructures. This allows not only bypassing difficulties in heteroepitaxy of lattice‐mismatched semiconductors of desired functionalities but also providing a scheme to design new optoelectronics that can surpass the fundamental limitations on their conventional semiconductor counterparts. Herein, a novel 2D h‐BN/p‐MoTe2/graphene/n‐SnS2/h‐BN p–g–n junction, fabricated by a layer‐by‐layer dry transfer, demonstrates high‐sensitivity, broadband photodetection at room temperature. The combination of the MoTe2 and SnS2 of complementary bandgaps, and the graphene interlayer provides a unique vdW heterostructure with a vertical built‐in electric field for high‐efficiency broadband light absorption, exciton dissociation, and carrier transfer. The graphene interlayer plays a critical role in enhancing sensitivity and broadening the spectral range. An optimized device containing 5?7‐layer graphene has been achieved and shows an extraordinary responsivity exceeding 2600 A W?1 with fast photoresponse and specific detectivity up to ≈1013 Jones in the ultraviolet–visible–near‐infrared spectrum. This result suggests that the vdW p–g–n junctions containing multiple photoactive TMDs can provide a viable approach toward future ultrahigh‐sensitivity and broadband photonic detectors.  相似文献   

2.
Van der Waals (vdW) epitaxy allows the fabrication of various heterostructures with dramatically released lattice matching conditions. This study demonstrates interface‐driven stacking boundaries in WS2 using epitaxially grown tungsten disulfide (WS2) on wrinkled graphene. Graphene wrinkles function as highly reactive nucleation sites on WS2 epilayers; however, they impede lateral growth and induce additional stress in the epilayer due to anisotropic friction. Moreover, partial dislocation‐driven in‐plane strain facilitates out‐of‐plane buckling with a height of 1 nm to release in‐plane strain. Remarkably, in‐plane strain relaxation at partial dislocations restores the bandgap to that of monolayer WS2 due to reduced interlayer interaction. These findings clarify significant substrate morphology effects even in vdW epitaxy and are potentially useful for various applications involving modifying optical and electronic properties by manipulating extended 1D defects via substrate morphology control.  相似文献   

3.
Optically generated excitonic states (excitons and trions) in transition metal dichalcogenides are highly sensitive to the electronic and magnetic properties of the materials underneath. Modulation and control of the excitonic states in a novel van der Waals (vdW) heterostructure of monolayer MoSe2 on double-layered perovskite Mn oxide ((La0.8Nd0.2)1.2Sr1.8Mn2O7) is demonstrated, wherein the Mn oxide transforms from a paramagnetic insulator to a ferromagnetic metal. A discontinuous change in the exciton photoluminescence intensity via dielectric screening is observed. Further, a relatively high trion intensity is discovered due to the charge transfer from metallic Mn oxide under the Curie temperature. Moreover, the vdW heterostructures with an ultrathin h-BN spacer layer demonstrate enhanced valley splitting and polarization of excitonic states due to the proximity effect of the ferromagnetic spins of Mn oxide. The controllable h-BN thickness in vdW heterostructures reveals a several-nanometer-long scale of charge transfer as well as a magnetic proximity effect. The vdW heterostructure allows modulation and control of the excitonic states via dielectric screening, charge carriers, and magnetic spins.  相似文献   

4.
Van der Waals (vdW) p–n heterojunctions consisting of various 2D layer compounds are fascinating new artificial materials that can possess novel physics and functionalities enabling the next‐generation of electronics and optoelectronics devices. Here, it is reported that the WSe2/WS2 p–n heterojunctions perform novel electrical transport properties such as distinct rectifying, ambipolar, and hysteresis characteristics. Intriguingly, the novel tunable polarity transition along a route of n‐“anti‐bipolar”–p‐ambipolar is observed in the WSe2/WS2 heterojunctions owing to the successive work of conducting channels of junctions, p‐WSe2 and n‐WS2 on the electrical transport of the whole systems. The type‐II band alignment obtained from first principle calculations and built‐in potential in this vdW heterojunction can also facilitate the efficient electron–hole separation, thus enabling the significant photovoltaic effect and a much enhanced self‐driven photoswitching response in this system.  相似文献   

5.
Heat dissipation is a major limitation of high-performance electronics. This is especially important in emerging nanoelectronic devices consisting of ultra-thin layers, heterostructures, and interfaces, where enhancement in thermal transport is highly desired. Here, ultra-high interfacial thermal conductance in encapsulated van der Waals (vdW) heterostructures with single-layer transition metal dichalcogenides MX2 (MoS2, WSe2, WS2) sandwiched between two hexagonal boron nitride (hBN) layers is reported. Through Raman spectroscopic measurements of suspended and substrate-supported hBN/MX2/hBN heterostructures with varying laser power and temperature, the out-of-plane interfacial thermal conductance in the vertical stack is calibrated. The measured interfacial thermal conductance between MX2 and hBN reaches 74 ± 25 MW m−2 K−1, which is at least ten times higher than the interfacial thermal conductance of MX2 in non-encapsulation structures. Molecular dynamics (MD) calculations verify and explain the experimental results, suggesting a full encapsulation by hBN layers is accounting for the high interfacial conductance. This ultra-high interfacial thermal conductance is attributed to the double heat transfer pathways and the clean and tight vdW interface between two crystalline 2D materials. The findings in this study reveal new thermal transport mechanisms in hBN/MX2/hBN structures and shed light on building novel hBN-encapsulated nanoelectronic devices with enhanced thermal management.  相似文献   

6.
Charge transfer in transition‐metal‐dichalcogenides (TMDs) heterostructures is a prerequisite for the formation of interlayer excitons, which hold great promise for optoelectronics and valleytronics. Charge accumulation accompanied by a charge‐transfer process can introduce considerable effect on interlayer exciton‐based applications; nevertheless, this aspect has been rarely studied up to date. This work demonstrates how the charge accumulation affects the light emission of interlayer excitons in van der Waals heterobilayers (HBs) consisting of monolayer WSe2 and WS2. As excitation power increases, the photoluminescence intensity of interlayer excitons increases more rapidly than that of intralayer excitons. The phenomenon can be explained by charge‐accumulation effect, which not only increases the recombination probability of interlayer excitons but also saturates the charge‐transfer process. This scenario is further confirmed by a careful examination of trion binding energy of WS2, which nonlinearly increases with the increase of the excitation power before reaching a maximum of about 75 meV. These investigations provide a better understanding of interlayer excitons and trions in HBs, which may provoke further explorations of excitonic physics as well as TMDs‐based devices.  相似文献   

7.
The 2D semiconductor monolayer transition metal dichalcogenides, WS2 and MoS2, are grown by chemical vapor deposition (CVD) and assembled by sequential transfer into vertical layered heterostructures (VLHs). Insulating hBN, also produced by CVD, is utilized to control the separation between WS2 and MoS2 by adjusting the layer number, leading to fine‐scale tuning of the interlayer interactions within the VLHs. The interlayer interactions are studied by photoluminescence (PL) spectroscopy and are demonstrated to be highly sensitive to the input excitation power. For thin hBN separators (one to two layers), the total PL emission switches from quenching to enhancement by increasing the laser power. Femtosecond broadband transient absorption measurements demonstrate that the increase in PL quantum yield results from Förster energy transfer from MoS2 to WS2. The PL signal is further enhanced at cryogenic temperatures due to the suppressed nonradiative decay channels. It is shown that (4 ± 1) layers of hBN are optimum for obtaining PL enhancement in the VLHs. Increasing thickness beyond this causes the enhancement factor to diminish, with the WS2 and MoS2 then behaving as isolated noninteracting monolayers. These results indicate how controlling the exciton generation rate influences energy transfer and plays an important role in the properties of VLHs.  相似文献   

8.
Semiconductor heterostructures have played a critical role as the enabler for new science and technology. The emergence of transition‐metal dichalcogenides (TMDs) as atomically thin semiconductors has opened new frontiers in semiconductor heterostructures either by stacking different TMDs to form vertical heterojunctions or by stitching them laterally to form lateral heterojunctions via direct growth. In conventional semiconductor heterostructures, the design of multijunctions is critical to achieve carrier confinement. Analogously, successful synthesis of a monolayer WS2/WS2(1?x )Se2x /WS2 multijunction lateral heterostructure via direct growth by chemical vapor deposition is reported. The grown structures are characterized by Raman, photoluminescence, and annular dark‐field scanning transmission electron microscopy to determine their lateral compositional profile. More importantly, using microwave impedance microscopy, it is demonstrated that the local photoconductivity in the alloy region can be tailored and enhanced by two orders of magnitude over pure WS2. Finite element analysis confirms that this effect is due to the carrier diffusion and confinement into the alloy region. This work exemplifies the technological potential of atomically thin lateral heterostructures in optoelectronic applications.  相似文献   

9.
Van der Waals (vdW) heterostructures combining layered ferromagnets and other 2D crystals are promising building blocks for the realization of ultracompact devices with integrated magnetic, electronic, and optical functionalities. Their implementation in various technologies depends strongly on the development of a bottom-up scalable synthesis approach allowing for realizing highly uniform heterostructures with well-defined interfaces between different 2D-layered materials. It is also required that each material component of the heterostructure remains functional, which ideally includes ferromagnetic order above room temperature for 2D ferromagnets. Here, it is demonstrated that the large-area growth of Fe5−xGeTe2/graphene heterostructures is achieved by vdW epitaxy of Fe5−xGeTe2 on epitaxial graphene. Structural characterization confirms the realization of a continuous vdW heterostructure film with a sharp interface between Fe5−xGeTe2 and graphene. Magnetic and transport studies reveal that the ferromagnetic order persists well above 300 K with a perpendicular magnetic anisotropy. In addition, epitaxial graphene on SiC(0001) continues to exhibit a high electronic quality. These results represent an important advance beyond nonscalable flake exfoliation and stacking methods, thus marking a crucial step toward the implementation of ferromagnetic 2D materials in practical applications.  相似文献   

10.
2D semiconducting transition metal dichalcogenides (TMDs) are endowed with fascinating optical properties especially in their monolayer limit. Insulating hBN films possessing customizable thickness can act as a separation barrier to dictate the interactions between TMDs. In this work, vertical layered heterostructures (VLHs) of WS2:hBN:WS2 are fabricated utilizing chemical vapor deposition (CVD)‐grown materials, and the optical performance is evaluated through photoluminescence (PL) spectroscopy. Apart from the prohibited indirect optical transition due to the insertion of hBN spacers, the variation in the doping level of WS2 drives energy transfer to arise from the layer with lower quantum efficiency to the other layer with higher quantum efficiency, whereby the total PL yield of the heterosystem is increased and the stack exhibits a higher PL intensity compared to the sum of those in the two WS2 constituents. Such doping effects originate from the interfaces that WS2 monolayers reside on and interact with. The electron density in the WS2 is also controlled and subsequent modulation of PL in the heterostructure is demonstrated by applying back‐gated voltages. Other influential factors include the strain in WS2 and temperature. Being able to tune the energy transfer in the VLHs may expand the development of photonic applications in 2D systems.  相似文献   

11.
Van der Waals (vdW) heterostructures have received intense attention for their efficient stacking methodology with 2D nanomaterials in vertical dimension. However, it is still a challenge to scale down the lateral size of vdW heterostructures to the nanometer and make proper contacts to achieve optimized performances. Here, a carbon‐nanotube‐confined vertical heterostructure (CCVH) is employed to address this challenge, in which 2D semiconductors are asymmetrically sandwiched by an individual metallic single‐walled carbon nanotube (SWCNT) and a metal electrode. By using WSe2 and MoS2, the CCVH can be made into p‐type and n‐type field effect transistors with high on/off ratios even when the channel length is 3.3 nm. A complementary inverter was further built with them, indicating their potential in logic circuits with a high integration level. Furthermore, the Fermi level of SWCNTs can be efficiently modulated by the gate voltage, making it competent for both electron and hole injection in the CCVHs. This unique property is shown by the transition of WSe2 CCVH from unipolar to bipolar, and the transition of WSe2/MoS2 from p–n junction to n–n junction under proper source–drain biases and gate voltages. Therefore, the CCVH, as a member of 1D/2D mixed heterostructures, shows great potentials in future nanoelectronics and nano‐optoelectronics.  相似文献   

12.
The field of photovoltaics is revolutionized in recent years by the development of two–dimensional (2D) type-II heterostructures. These heterostructures are made up of two different materials with different electronic properties, which allows for the capture of a broader spectrum of solar energy than traditional photovoltaic devices. In this study, the potential of vanadium (V)-doped WS2 is investigated, hereafter labeled V-WS2, in combination with air-stable Bi2O2Se for use in high-performance photovoltaic devices. Various techniques are used to confirm the charge transfer of these heterostructures, including photoluminescence (PL) and Raman spectroscopy, along with Kelvin probe force microscopy (KPFM). The results show that the PL is quenched by 40%, 95%, and 97% for WS2/Bi2O2Se, 0.4 at.% V-WS2/Bi2O2Se, and 2 at.% V-WS2/Bi2O2Se, respectively, indicating a superior charge transfer in V-WS2/Bi2O2Se compared to pristine WS2/Bi2O2Se. The exciton binding energies for WS2/Bi2O2Se, 0.4 at.% V-WS2/Bi2O2Se and 2 at.% V-WS2/Bi2O2Se heterostructures are estimated to be ≈130, 100, and 80 meV, respectively, which is much lower than that for monolayer WS2. These findings confirm that by incorporating V-doped WS2, charge transfer in WS2/Bi2O2Se heterostructures can be tuned, providing a novel light-harvesting technique for the development of the next generation of photovoltaic devices based on V-doped transition metal dichalcogenides (TMDCs)/Bi2O2Se.  相似文献   

13.
Van der Waals (vdW) heterostructures, which have the advantage of integrating excellent properties of the stacked 2D materials by vdW interactions, have gained increasing attention recently. In this work, within the framework of density functional theory calculations, the electronic properties of vdW heterostructure composed of phosphorene (BP) in black phosphorus phase and GeS monolayer are systematically explored. The results show that the carriers are not separated for both lattice‐match and lattice‐mismatch heterostructures. For the lattice‐match heterostructure, it is found that changing monolayer of GeS to bilayer can increase the energy difference of valence band offsets between GeS and BP, thus realizing electron–hole separation. For the lattice‐mismatch heterostructure, altering the layer distance can transform the heterostructure into a typical type‐I alignment, but applying the electric field or doping with 2, 3, 5, 6‐tetrafluoro‐7, 7, 8, 8‐tetracyanoquinodimethane (F4TCNQ) can make it display a perfect desirable type‐II alignment, where holes migration and electrons transfer are revealed to account respectively for the phenomenon of carrier separation. It is believed that the work would greatly enlarge the potential application of the BP‐based heterostructures in photoelectronics and further stimulate the investigation enthusiasms on other fashionable heterostructures and even unassuming heterostructures in which the charming electronic properties can be modulated to emerge by various general methods.  相似文献   

14.
Design and synthesis of ordered, metal‐free layered materials is intrinsically difficult due to the limitations of vapor deposition processes that are used in their making. Mixed‐dimensional (2D/3D) metal‐free van der Waals (vdW) heterostructures based on triazine (C3N3) linkers grow as large area, transparent yellow‐orange membranes on copper surfaces from solution. The membranes have an indirect band gap (E g,opt = 1.91 eV, E g,elec = 1.84 eV) and are moderately porous (124 m2 g?1). The material consists of a crystalline 2D phase that is fully sp2 hybridized and provides structural stability, and an amorphous, porous phase with mixed sp2–sp hybridization. Interestingly, this 2D/3D vdW heterostructure grows in a twinned mechanism from a one‐pot reaction mixture: unprecedented for metal‐free frameworks and a direct consequence of on‐catalyst synthesis. Thanks to the efficient type I heterojunction, electron transfer processes are fundamentally improved and hence, the material is capable of metal‐free, light‐induced hydrogen evolution from water without the need for a noble metal cocatalyst (34 µmol h?1 g?1 without Pt). The results highlight that twinned growth mechanisms are observed in the realm of “wet” chemistry, and that they can be used to fabricate otherwise challenging 2D/3D vdW heterostructures with composite properties.  相似文献   

15.
Vertically stacked van der Waals (vdW) heterostructures have been suggested as a robust platform for studying interfacial phenomena and related electric/optoelectronic devices. While the interlayer Coulomb interaction mediated by the vdW coupling has been extensively studied for carrier recombination processes in a diode transport, its correlation with the interlayer tunneling transport has not been elucidated. Here, a contrast is reported between tunneling and drift photocurrents tailored by the interlayer coupling strength in MoSe2/MoS2 hetero‐bilayers (HBs). The interfacial coupling modulated by thermal annealing is identified by the interlayer phonon coupling in Raman spectra and the emerging interlayer exciton peak in photoluminescence spectra. In strongly coupled HBs, positive photocurrents are observed owing to the inelastic band‐to‐band tunneling assisted by interlayer excitons that prevail over exciton recombinations. By contrast, weakly coupled HBs exhibit a negative photovoltaic diode behavior, manifested as a drift current without interlayer excitonic emissions. This study sheds light on tailoring the tunneling transport for numerous optoelectronic HB devices.  相似文献   

16.
Transition metal dichalcogenides (TMDs) van der Waals (vdW) 1D heterostructures are recently synthesized from 2D nanosheets, which open up new opportunities for potential applications in electronic and optoelectronic devices. The most recent and promising strategies in regards to forming 1D TMDs nanotubes (NTs) or nanoscrolls (NSs) in this review article as well as their heterostructures that are produced from 2D TMDs are summarized. In order to improve the functionality of ultrathin 1D TMDs that are coaxially combined with boron nitride nanotubes and single-walled carbon nanotubes. 1D heterostructured devices perform better than 2D TMD nanosheets when the two devices are compared. The photovoltaic effect in WS2 or MoS2 NTs without a junction may exceed the Shockley–Queisser limit for the above-band-gap photovoltage generation. Photoelectrochemical hydrogen evolution is accelerated when monolayer WS2 or MoS2 NSs are incorporated into a heterojunction. In addition, the photovoltaic performance of the WSe2/MoS2 NSs junction is superior to that of the performance of MoS2 NSs. The summary of the current research about 1D TMDs can be used in a variety of ways, which assists in the development of new types of nanoscale optoelectronic devices. Finally, it also summarizes the current challenges and prospects.  相似文献   

17.
Heterostructured materials integrate the advantages of adjustable electronic structure, fast electron/ions transfer kinetics, and robust architectures, which have attracted considerable interest in the fields of rechargeable batteries, photo/electrocatalysis, and supercapacitors. However, the construction of heterostructures still faces some severe problems, such as inferior random packing of components and serious agglomeration. Herein, a terminal group-oriented self-assembly strategy to controllably synthesize a homogeneous layer-by-layer SnSe2 and MXene heterostructure (LBL-SnSe2@MXene) is designed. Benefitting from the abundant polar terminal groups on the MXene surface, Sn2+ is induced into the interlayer of MXene with large interlayer spacing, which is selenized in situ to obtain LBL-SnSe2@MXene. In the heterostructure, SnSe2 layers and MXene layers are uniformly intercalated in each other, superior to other heterostructures formed by random stacking. As an anode for lithium-ion batteries, the LBL-SnSe2@MXene is revealed to possess strong lithium adsorption ability, the small activation energy for lithium diffusion, and excellent structure stability, thus achieving outstanding electrochemical performance, especially with high specific capacities (1311 and 839 mAh g−1 for initial discharge and charge respectively) and ultralong cycling stability (410 mAh g−1 at 5C even after 16 000 cycles). This work conveys an inspiration for the controllable design and construction of homogeneous layered heterostructures.  相似文献   

18.
2D metal‐semiconductor heterostructures based on transition metal dichalcogenides (TMDs) are considered as intriguing building blocks for various fields, such as contact engineering and high‐frequency devices. Although, a series of p–n junctions utilizing semiconducting TMDs have been constructed hitherto, the realization of such a scheme using 2D metallic analogs has not been reported. Here, the synthesis of uniform monolayer metallic NbS2 on sapphire substrate with domain size reaching to a millimeter scale via a facile chemical vapor deposition (CVD) route is demonstrated. More importantly, the epitaxial growth of NbS2‐WS2 lateral metal‐semiconductor heterostructures via a “two‐step” CVD method is realized. Both the lateral and vertical NbS2‐WS2 heterostructures are achieved here. Transmission electron microscopy studies reveal a clear chemical modulation with distinct interfaces. Raman and photoluminescence maps confirm the precisely controlled spatial modulation of the as‐grown NbS2‐WS2 heterostructures. The existence of the NbS2‐WS2 heterostructures is further manifested by electrical transport measurements. This work broadens the horizon of the in situ synthesis of TMD‐based heterostructures and enlightens the possibility of applications based on 2D metal‐semiconductor heterostructures.  相似文献   

19.
Semiconductor-based heterostructures have exhibited great promise as a photocatalyst to convert solar energy into sustainable chemical fuels, however, their solar-to-fuel efficiency is largely restricted by insufficient interfacial charge separation and limited catalytically active sites. Here the integration of high-efficiency interfacial charge separation and sufficient single-atom metal active sites in a 2D van der Waals (vdW) heterostructure between ultrathin polymeric carbon nitride (p-CN) and Ni-containing Salphen-based covalent organic framework (Ni-COF) nanosheets is illustrated. The results reveal a Ni N2 O2 chemical bonding in NiCOF nanosheets, leading to a highly separated single-atom Ni sites, which will function as the catalytically active sites to boost solar fuel production, as confirmed by X-ray absorption spectra and density functional theory calculations. Using ultrafast femtosecond transient adsorption (fs-TA) spectra, it shows that the vdW p-CN/Ni-COF heterostructure exhibits a faster decay lifetime of the exciton annihilation (τ = 18.3 ps) compared to that of neat p-CN (32.6 ps), illustrating an efficiently accelerated electron transfer across the vdW heterointerface from p-CN to Ni-COF, which thus allows more active electrons available to participate in the subsequent reduction reactions. The photocatalytic results offer a chemical fuel generation rate of 2.29 mmol g−1 h−1 for H2 and 6.2 µmol g−1 h−1 for CO, ≈127 and three times higher than that of neat p-CN, respectively. This work provides new insights into the construction of a π-conjugated vdW heterostructure on promoting interfacial charge separation for high-efficiency photocatalysis.  相似文献   

20.
Dirac semimetal is an emerging class of quantum matters, ranging from 2D category, such as, graphene and surface states of topological insulator to 3D category, for instance, Cd3As2 and Na3Bi. As 3D Dirac semimetals typically possess Fermi‐arc surface states, the 2D–3D Dirac van der Waals heterostructures should be promising for future electronics. Here, graphene–Cd3As2 heterostructures are fabricated through direct layer‐by‐layer stacking. The electronic coupling results in a notable interlayer charge transfer, which enables us to modulate the Fermi level of graphene through Cd3As2. A planar graphene p–n–p junction is achieved by selective modification, which demonstrates quantized conductance plateaus. Moreover, compared with the bare graphene device, the graphene–Cd3As2 hybrid device presents large nonlocal signals near the Dirac point due to the charge transfer from the spin‐polarized surface states in the adjacent Cd3As2. The results enrich the family of van der Waals heterostructure and should inspire more studies on the application of Dirac/Weyl semimetals in spintronics.  相似文献   

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