Devices and applications of van der Waals heterostructures

Van der Waals heterostructures, composed of individual two-dimensional material have been developing extremely fast. Synthesis of van der Waals heterostructures without the constraint of lattice matching and processing compatibility provides an ideal platform for fundamental research and new device exploitation. We review the approach of synthesis of van der Waals heterostructures, discuss the property of heterostructures and thoroughly illustrate the functional van der Waals heterostructures used in novel electronic and photoelectronic device.     

Giant and Nonvolatile Control of Exchange Bias in Fe3GeTe2/Irradiated Fe3GeTe2/MgO Heterostructure Through Ultralow Voltage

The discovery of van der Waals magnets has provided a new platform for the electrical control of magnetism. Recent experiments have demonstrated that the magnetic properties of van der Waals magnets can be tuned by various gate modulations, although most of them are volatile and require gate voltages no lower than several volts. Here, the realization of nonvolatile control of exchange bias and coercive fields in Fe₃GeTe₂/MgO heterostructures, and the gate voltage is as low as tens of mV which is two orders of magnitude smaller than those in previous experiments is presented. The discovery of an ionic-irradiated phase formed in Fe₃GeTe₂ by MgO sputtering revealed that an exchange bias effect can be obtained in this heterostructure and tuned from ≈700 to 0 Oe through voltages ranging from 5 to 20 mV. Owing to the high stability of oxidized Fe₃GeTe₂, the voltage-driven oxygen incorporated into Fe₃GeTe₂ from the irradiated phase induces a nonvolatile magnetism modulation that can be retained after turning off the gate voltage. These findings demonstrate a methodology to modulate the magnetism of van der Waals magnets, opening new opportunities to fabricate all-solid, long-retention, and low-dissipation nano-electronic devices using van der Waals materials.     

Two‐Dimensional Magnets: Forgotten History and Recent Progress towards Spintronic Applications

The recent discovery of 2D magnetic order in van der Waals materials has stimulated a renaissance in the field of atomically thin magnets. This has led to promising demonstrations of spintronic functionality such as tunneling magnetoresistance. The frantic pace of this emerging research, however, has also led to some confusion surrounding the underlying phenomena of phase transitions in 2D magnets. In fact, there is a rich history of experimental precedents beginning in the 1960s with quasi‐2D bulk magnets and progressing to the 1980s using atomically thin sheets of elemental metals. This review provides a holistic discussion of the current state of knowledge on the three distinct families of low‐dimensional magnets: quasi‐2D, ultrathin films, and van der Waals crystals. It highlights the unique opportunities presented by the latest implementation in van der Waals materials. By revisiting the fundamental insights from the field of low‐dimensional magnetism, this review highlights factors that can be used to enhance material performance. For example, the limits imposed on the critical temperature by the Mermin–Wagner theorem can be escaped in three separate ways: magnetocrystalline anisotropy, long‐range interactions, and shape anisotropy. Several recent experimental reports of atomically thin magnets with Curie temperatures above room temperature are highlighted.     

Manipulation of Magnetic Skyrmion in a 2D van der Waals Heterostructure via Both Electric and Magnetic Fields

As a promising candidate for the much-desired low power consumption spintronic devices, 2D magnetic van der Waals material also provides a versatile platform for the design and control of topological spin textures. In this work on WTe₂/CrCl₃ bilayer van der Waals heterostructures, a complete Néel-type skyrmion–bimeron–ferromagnet phase transition is demonstrated, accompanied by the evolution of the topological number. This cyclic transition, mediated by a perpendicular magnetic field, is largely driven by the competition between the out-of-plane magnetocrystalline anisotropy and magnetic dipole–dipole interaction. In the presence of a driving current, the Néel-type skyrmion gains a higher velocity yet larger skyrmion Hall angle, in comparison to the bimeron. By incorporating a ferroelectric CuInP₂S₆ monolayer as a substrate, writing and erasing of skyrmions may be regulated using a ferroelectric polarization. This work sheds light on a novel approach to the design and control of magnetic skyrmions on 2D van der Waals materials.     

Modeling the Transport Properties of a 1D van der Waals Heterojunction Formed by a Carbon Nanotube and a MoS2 Nanotube

Semiconductors - 2D layered materials can be combined for heterogeneous integration at the atomic level without the lattice-matching limitation due to the concept of van der Waals heterostructures....     

2D van der Waals Heterojunction Nanophotonic Devices: From Fabrication to Performance

2D van der Waals heterojunctions (vdWhs) are a novel type of metamaterial that are flexible, adjustable, and easy to assemble. Using weak van der Waals forces (vdWfs), layered 2D materials can stack freely to form vdWhs with atomic level flat interfaces. By using different 2D materials and specific stacking methods, their unique properties can be organically combined, to exhibit more abundant optical properties. In fact, nanophotonic devices based on 2D vdWhs have developed rapidly and made significant progress. Therefore, the main progress of 2D vdWhs nanophotonic devices in recent years, including the preparation methods of 2D vdWhs and the performance improvements of various nanophotonic devices, is reviewed. Lastly, the prospects of 2D vdWhs nanophotonic devices are discussed.     

MoS2 Van der Waals p–n Junctions Enabling Highly Selective Room‐Temperature NO2 Sensor

Van der Waals p–n junctions of 2D materials present great potential for electronic devices due to the fascinating properties at the junction interface. In this work, an efficient gas sensor based on planar 2D van der Waals junctions is reported by stacking n‐type and p‐type atomically thin MoS₂ films, which are synthesized by chemical vapor deposition (CVD) and soft‐chemistry route, respectively. The electrical conductivity of the van der Waals p–n junctions is found to be strongly affected by the exposure to NO₂ at room temperature (RT). The MoS₂ p–n junction sensor exhibits an outstanding sensitivity and selectivity to NO₂ at RT, which are unavailable in sensors based on individual n‐type or p‐type MoS₂. The sensitivity of 20 ppm NO₂ is improved by 60 times compared to a p‐type MoS₂ sensor, and an extremely low limit of detection of 8 ppb is obtained under ultraviolet irradiation. Complete and very fast sensor recovery is achieved within 30 s. These results are superior to most of the previous reports related to NO₂ detection. This work establishes an entirely new sensing platform and proves the feasibility of using such materials for the high‐performance detection of gaseous molecules at RT.     

Ultrathin Non‐van der Waals Magnetic Rhombohedral Cr2S3: Space‐Confined Chemical Vapor Deposition Synthesis and Raman Scattering Investigation

Two dimensional (2D) magnetic materials display enormous application potential in spintronic fields. However, most of currently reported magnetic materials are van der Waals layered structure that is easy to be isolated via exfoliation method. By contrast, the studies on non‐van der Waals ultrathin magnetic materials are rare, largely due to the difficulty in fabrication. Rhombohedral Cr₂S₃, an intensively studied antiferromagnetic transition metal chalcogenide with Neel temperature of ≈120 K, has a typical non‐van der Waals structure. Restricted by the strong covalent bonding in all the three dimensions of non‐van der Waals structure, the synthesis of ultrathin Cr₂S₃ single crystals is still a challenge that is not achieved yet. Besides, the study on the Raman modes of rhombohedral Cr₂S₃ is also absent. Herein, by employing space‐confined chemical vapor deposition strategy, ultrathin rhombohedral Cr₂S₃ single crystals with a thickness down to ≈2.5 nm for the first time are successfully grown. Moreover, a systematically investigation is also conducted on the Raman vibrations of ultrathin rhombohedral Cr₂S₃. With the aid of angle‐resolved polarized Raman technique, the Raman modes of rhombohedral Cr₂S₃ for the first time based on crystal symmetry and Raman selection rules are rationally assigned.     

AsP/InSe Van der Waals Tunneling Heterojunctions with Ultrahigh Reverse Rectification Ratio and High Photosensitivity

Van der Waals heterojunctions made of 2D materials offer competitive opportunities in designing and achieving multifunctional and high‐performance electronic and optoelectronic devices. However, due to the significant reverse tunneling current in such thin p–n junctions, a low rectification ratio along with a large reverse current is often inevitable for the heterojunctions. Here, a vertically stacked van der Waals heterojunction (vdWH) tunneling device is reported consisting of black arsenic phosphorus (AsP) and indium selenide (InSe), which shows a record high reverse rectification ratio exceeding 10⁷ along with an unusual ultralow forward current below picoampere and a high current on/off ratio over 10⁸ simultaneously at room temperature under the proper band alignment design of both the Schottky junction and the heterojunction. Therefore, the vdWH tunneling device can function as an ultrasensitive photodetector with an ultrahigh light on/off ratio of 1 × 10⁷, a comparable responsivity of around 1 A W^?1, and a high detectivity over 1 × 10¹² Jones in the visible wavelength range. Furthermore, the device exhibits a clear photovoltaic effect and shows a spectral detection capability up to 1550 nm. The work sheds light on developing future electronic and optoelectronic multifunctional devices based on the van der Waals integration of 2D materials with designed band alignment.     

Two-dimensional air-stable CrSe2 nanosheets with thickness-tunable magnetism

Since Geim et al.firstly separated graphene from graph-ite by mechanical exfoliation method in 2004,the research of two-dimensional (2D) van der Waals (vdW) layered materials has begun[1].Compared with three-dimensional materials,2D vdW layered materials exposing the most atoms to exterior are more sensitive to external control and have the great po-tential applications in electronic,optoelectronic and electro-chemical area[2].     

Layer-number dependent high-frequency vibration modes in few-layer transition metal dichalcogenides induced by interlayer couplings

Two-dimensional transition metal dichalcogenides (TMDs) have attracted extensive attention due to their many novel properties. The atoms within each layer in two-dimensional TMDs are joined together by covalent bonds, while van der Waals interactions combine the layers together. This makes its lattice dynamics layer-number dependent. The evolutions of ultralow frequency (<50 cm^-1) modes, such as shear and layer-breathing modes have been well-established. Here, we review the layer-number dependent high-frequency (>50 cm^-1) vibration modes in few-layer TMDs and demonstrate how the interlayer coupling leads to the splitting of high-frequency vibration modes, known as Davydov splitting. Such Davydov splitting can be well described by a van der Waals model, which directly links the splitting with the interlayer coupling. Our review expands the understanding on the effect of interlayer coupling on the high-frequency vibration modes in TMDs and other two-dimensional materials.     

Van der Waals Nanowires with Continuously Variable Interlayer Twist and Twist Homojunctions

Moiré patterns at van der Waals interfaces between twisted 2D crystals give rise to distinct optoelectronic excitations, as well as, narrowly dispersive bands responsible for correlated electron phenomena. Contrasting with the conventional, mechanically stacked planar twist moirés, recent work shows twisted van der Waals interfaces spontaneously formed in nanowires of layered crystals, where Eshelby twist due to axial screw dislocations stabilizes a chiral structure with small interlayer rotation. Here, the realization of tunable twist in germanium(II) sulfide (GeS) van der Waals nanowires is reported. Tapered nanowires host continuously variable interlayer twist. Homojunctions between dislocated (chiral) and defect-free (achiral) segments are obtained by triggering the emission of axial dislocations during growth. Measurements across such junctions, implemented here using local absorption and luminescence spectroscopy, provide a convenient tool for detecting twist effects. The results identify a versatile system for 3D twistronics, probing moiré physics, and for realizing moiré architectures without equivalent in planar systems.     

InSe Schottky Diodes Based on Van Der Waals Contacts

2D semiconductors are excellent candidates for next‐generation electronics and optoelectronics thanks to their electrical properties and strong light‐matter interaction. To fabricate devices with optimal electrical properties, it is crucial to have both high‐quality semiconducting crystals and ideal contacts at metal‐semiconductor interfaces. Thanks to the mechanical exfoliation of van der Waals crystals, atomically thin high‐quality single‐crystals can easily be obtained in a laboratory. However, conventional metal deposition techniques can introduce chemical disorder and metal‐induced mid‐gap states that induce Fermi level pinning and can degrade the metal‐semiconductor interfaces, resulting in poorly performing devices. In this article, the electrical contact characteristics of Au–InSe and graphite–InSe van der Waals contacts, obtained by stacking mechanically exfoliated InSe flakes onto pre‐patterned Au or graphite electrodes without the need for lithography or metal deposition is explored. The high quality of the metal‐semiconductor interfaces obtained by van der Waals contact allows to fabricate high‐quality Schottky diodes based on the Au–InSe Schottky barrier. The experimental observation indicates that the contact barrier at the graphite–InSe interface is negligible due to the similar electron affinity of InSe and graphite, while the Au–InSe interfaces are dominated by a large Schottky barrier.     

Visualizing Energy Transfer at Buried Interfaces in Layered Materials Using Picosecond X‐Rays

Understanding the fundamentals of nanoscale heat propagation is crucial for next‐generation electronics. For instance, weak van der Waals bonds of layered materials are known to limit their thermal boundary conductance (TBC), presenting a heat dissipation bottleneck. Here, a new nondestructive method is presented to probe heat transport in nanoscale crystalline materials using time‐resolved X‐ray measurements of photoinduced thermal strain. This technique directly monitors time‐dependent temperature changes in the crystal and the subsequent relaxation across buried interfaces by measuring changes in the c‐axis lattice spacing after optical excitation. Films of five different layered transition metal dichalcogenides MoX₂ [X = S, Se, and Te] and WX₂ [X = S and Se] as well as graphite and a W‐doped alloy of MoTe₂ are investigated. TBC values in the range 10–30 MW m^?2 K^?1 are found, on c‐plane sapphire substrates at room temperature. In conjunction with molecular dynamics simulations, it is shown that the high thermal resistances are a consequence of weak interfacial van der Waals bonding and low phonon irradiance. This work paves the way for an improved understanding of thermal bottlenecks in emerging 3D heterogeneously integrated technologies.     

van der Waals Epitaxial Growth of Atomically Thin 2D Metals on Dangling‐Bond‐Free WSe2 and WS2

2D metals have attracted considerable recent attention for their special physical properties, such as charge density waves, magnetism, and superconductivity. However, despite some recent efforts, the synthesis of ultrathin 2D metals nanosheets down to monolayer thickness remains a significant challenge. Herein, by using atomically flat 2D WSe₂ or WS₂ as the growth substrate, the synthesis of atomically thin 2D metallic MTe₂ (M = V, Nb, Ta) single crystals with the thickness down to the monolayer regime and the creation of atomically thin MTe₂/WSe₂ (WS₂) vertical heterojunctions is reported. Comparison with the growth on the SiO₂/Si substrate under the same conditions reveals that the utilization of the dangling‐bond‐free WSe₂ or WS₂ as the van der Waals epitaxy substrates is crucial for the successful realization of atomically thin MTe₂ (M = V, Nb, Ta) nanosheets. It is further shown that the epitaxial grown 2D metals can function as van der Waals contacts for 2D semiconductors with little interface damage and improved electronic performance. This study defines a robust van der Waals epitaxy pathway to ultrathin 2D metals, which is essential for fundamental studies and potential technological applications of this new class of materials at the 2D limit.     

利用低温生长法制备水纳米团簇和二维冰

利用低温扫描隧道显微镜(LT?STM)研究了水分子在高定向裂解石墨(HOPG)表面的低温吸附和薄膜生长.在低覆盖度下,水分子在HOPG表面会形成二聚体,三聚体,甚至更大的自组装纳米团簇.在高覆盖度下,水分子形成单分子层厚的二维水膜,其面内结构是非共边的六边形蜂窝状结构,类似于体材料的Ice?Ⅱ相.通过傅里叶变换和莫尔条纹分析,本文发现水膜和HOPG衬底之间存在不同的夹角,表明分子-衬底之间的相互作用很弱.     

Mo6S3Br6: An Anisotropic 2D Superatomic Semiconductor

Two‐dimensional (2D) van der Waals materials with in‐plane anisotropy are of great interest for directional transport of charge and energy, as exemplified by recent studies on black phosphorus and α‐phase molybdenum trioxide (α‐MO₃). Here, a layered van der Waals semiconductor with in‐plane anisotropy built upon the superatomic units of Mo₆S₃Br₆ is reported. This material possesses robust 2D characteristics with a direct gap of 1.64 eV, as determined by scanning tunneling spectroscopy and first‐principles calculations. Polarization‐dependent Raman spectroscopy measurement and density functional theory calculation reveal strong in‐plane anisotropy. These results suggest an effective strategy to explore anisotropic 2D electronic and optoelectronic properties from superatomic building blocks with multifunctionality, emergent properties, and hierarchical control.     

Van der Waals Heterostructure Devices with Dynamically Controlled Conduction Polarity and Multifunctionality

Controlling the conduction behavior of 2D materials is an important prerequisite to achieve their electronic and optoelectronic applications. However, most of the reported approaches are aware of the shortcomings of inflexibility and complexity, which limits the possibility of multifunctional integration. Here, taking advantage of van der Waals heterostructure engineering, a simple method to achieve a dynamically controlled binary channel in a semivertical MoTe₂/MoS₂ field effect transistor is proposed. It is enabled by the high switchability between tunneling and thermal transports through simply changing the sign of voltage bias. In addition, the proposed system allows for multifunctional integration of transistor with on/off ratio >10⁷ and diode with rectification ratio >10⁶. Moreover, the devices show screen capability to negative photoresponse effect that is widely observed in ambipolar materials, hence improving the photodetection reliability and sensitivity. This study broadens the functionalities of van der Waals heterostructures and opens up more possibilities to realize multifunctional devices.     

Enhanced Thermal Transport across Self-Interfacing van der Waals Contacts in Flexible Thermal Devices

Minimizing the thermal contact resistance (TCR) at the boundary between two bodies in contact is critical in diverse thermal transport devices. Conventional thermal contact methods have several limitations, such as high TCR, low interfacial adhesion, a requirement for high external pressure, and low optical transparency. Here, a self-interfacing flexible thermal device (STD) that can form robust van der Waals mechanical contact and low-resistant thermal contact to planar and non-planar substrates without the need for external pressure or surface modification is presented. The device is based on a distinctive integration of a bioinspired adhesive architecture and a thermal transport layer formed from percolating silver nanowire (AgNW) networks. The proposed device exhibits a strong attachment (maximum 538.9 kPa) to target substrates while facilitating thermal transport across the contact interface with low TCR (0.012 m² K kW⁻¹) without the use of external pressure, thermal interfacial materials, or surface chemistries.     

Electrical Conduction at the Interface between Insulating van der Waals Materials

Emergent properties of 2D materials attract considerable interest in condensed matter physics and materials science due to their distinguished features that are missing in their bulk counterparts. A mainstream in this research field is to broaden the scope of material to expand the horizons of the research area, while developing functional interfaces between different 2D materials is another indispensable research direction. Here, the emergence of electrical conduction at the interface between insulating 2D materials is demonstrated. A new class of van der Waals heterostructures consisting of two sets of insulating transition‐metal dichalcogenides, group‐VI WSe₂ and group‐IV TMSe₂ (TM = Zr, Hf), is developed via molecular‐beam epitaxy, and it is found that those heterostructures are highly conducting although all the constituent materials are highly insulating. The WSe₂/ZrSe₂ interface exhibits more conducting behavior than the WSe₂/HfSe₂ interface, which can be understood by considering the band alignments between constituent materials. Moreover, by increasing Se flux during heterostructure fabrication, the WSe₂/ZrSe₂ interface becomes more conducting, reaching nearly metallic behavior. Further improvement of the crystalline quality as well as exploring different material combinations are expected to lead to metallic conduction, providing a novel functionality emerging at van der Waals heterostructures.