The Anderson and midgap models are often used in the study of semiconductor heterojunctions, but for van der Waals (vdW) vertical heterostructures they have shown only very limited success. Using the group-IV monochalcogenide vertical heterostructures as a prototypical system, we propose a linear response model and compare the effectiveness of these models in predicting density functional theory (DFT) band alignments, band types and bandgaps. We show that the DFT band alignment is best predicted by the linear response model, which falls in between the Anderson and midgap models. Our proposed model can be characterized by an interface dipole $α\times(E_{m2}-E_{m1})$, where the linear response coefficient $α$ = 0 and 1 corresponds to the Anderson and midgap model respectively, and $E_{m}$ is the midgap energy of the monolayer, which can be viewed as an effective electronegativity. For group-IV monochalcogenides, we show that $α$ = 0.34 best captures the DFT band alignment of the vdW heterostructure, and we discuss the viability of the linear response model considering other effects such as strains and band hybridization, and conclude with an application of the model to predict experimental band alignments.
We present a model for P-N-P abrupt heterostructures vertical to temperature gradient to improve the thermoelectric performance. The P-N-P heterostructure is considered as an abrupt bipolar junction transistor due to an externally applied temperature gradient paralleled to depletion layers. Taking Bi2Te3 and Bi0.5Sb1.5Te3 as N-type and P-type thermoelectric materials respectively for example, we achieve the purpose of controlling the Seebeck coefficient and the electrical conductivity independently while amplifying operation power. The calculated results show that the Seebeck coefficient can r…
A novel vertical hysteresis loop shift is observed for a bilayer thin film of Ni80Fe20/SrRuO3 (1:2 thickness ratio) on SrTiO3 substrate, after field cooled through the Curie temperature ~125 K of SrRuO3, whereas no shift is found for zero field cooled measurement. The vertical shift is noticed below ~125 K which increases with decreasing temperature and reaches a maximum of 33% at 2 K. The vertical shift is modelled closely using micromagnetic simulations. It is shown that the amount of vertical shift depends on the competition between the relative thicknesses and the anisotropies of the two f…
Bulk photovoltaic (BPVE) effect in crystals lacking inversion symmetry offers great potential for optoelectronic applications due to its unique properties such as above bandgap photovoltage and switchable photocurrent. Because of their large spontaneous polarizations, ferroelectric materials are ideal platforms for studying BPVE. However, identifying the origin of experimentally observed photovoltaic response is often challenging due to the entanglement between bulk and interface effects, leading to much debate in the field. This issue is particularly pronounced in vertical heterostructures, w…
In integrating topological insulators (TIs) with conventional materials, one crucial issue is how the topological surface states (TSS) will behave in such heterostructures. We use first-principles approaches to establish accurate tunability of the vertical location of the TSS via intriguing dual-proximity effects. By depositing a conventional insulator (CI) overlayer onto a TI substrate (Bi2Se3 or Bi2Te3), we demonstrate that, the TSS can float to the top of the CI film, or stay put at the CI/TI interface, or be pushed down deeper into the otherwise structurally homogeneous TI substrate. These…
In this letter, we report on unipolar vertical transport characteristics in c-plane GaN/AlGaN/GaN heterostructures. Vertical current in heterostructures with random alloy barriers was found to be independent of dislocation density and heterostructure barrier height, and significantly higher than theoretical estimates. Percolation-based transport due to random alloy fluctuations in the ternary AlGaN is suggested as the dominant transport mechanism, and confirmed through experiments showing that non-random or digital AlGaN alloys and polarization-engineered binary GaN barriers can eliminate perc…
Low-dimensional metal-semiconductor vertical heterostructures (VH) are promising candidates in the search of electronic devices at the extreme limits of miniaturization. Within this line of research, here we present a theoretical/computational study of the NbS$_2$/WSe$_2$ metal-semiconductor vertical hetero-junction using density functional theory (DFT) and conductance simulations. We first construct atomistic models of the NbS$_2$/WSe$_2$ VH considering all the five possible stacking orientations at the interface, and we conduct DFT and quantum-mechanical (QM) scattering simulations to obtain…
The stacked two layered materials with a lattice constant mismatch and/or with twist angle relative to each other can create a moiré pattern, modulating the electronic properties of the pristine materials. Here, we combine scanning tunneling microscopy/spectroscopy and density functional theory calculations to investigate the moiré potential induced bandgap tuning in InSe/CuSe vertical heterostructure synthesized by a two-step of molecular beam epitaxy. Scanning tunneling microscopy measurements demonstrate the heterostructure with a superlattice periodicity of ~3.48nm and a twist angle of abo…
The metal-insulator transition (MIT) is one of the remarkable electrical transport properties of atomically thin molybdenum disulphide (MoS2). Although the theory of electron-electron interactions has been used in modeling the MIT phenomena in MoS2, the underlying mechanism and detailed MIT process still remain largely unexplored. Here, we demonstrate that the vertical metal-insulator-semiconductor (MIS) heterostructures built from atomically thin MoS2 (monolayers and multilayers) are ideal capacitor structures for probing the electron states in MoS2. The vertical configuration of MIS heterost…
We report a bipolar field effect tunneling transistor that exploits to advantage the low density of states in graphene and its one atomic layer thickness. Our proof-of-concept devices are graphene heterostructures with atomically thin boron nitride acting as a tunnel barrier. They exhibit room temperature switching ratios ~50, a value that can be enhanced further by optimizing the device structure. These devices have potential for high frequency operation and large scale integration.
We investigated the electronic and optoelectronic properties of vertical van der Waals heterostructure photodetectors using layered p type GaSe and n type InSe, with graphene as the transparent electrodes. Not only the photocurrent peaks from the layered GaSe and InSe themselves were observed, also the interlayer optical transition peak was observed, which is consistent with the first-principles calculation. The built-in electric field between p-n heterojunction and the advantage of the graphene electrodes can effectively separate the photo-induced electron-hole pairs, and thus lead to the res…
We report a buried heterostructure vertical-cavity surface-emitting laser fabricated by epitaxial regrowth over an InGaAs quantum well gain medium. The regrowth technique enables microscale lateral confinement that preserves a high cavity quality factor (loaded $Q\approx$ 4000) and eliminates parasitic charging effects found in existing approaches. Under optimal spectral overlap between gain medium and cavity mode (achieved here at $T$ = 40 K) lasing was obtained with an incident optical power as low as $P_{\rm th}$ = 10 mW ($λ_{\rm p}$ = 808 nm). The laser linewidth was found to be $\approx$3…
Vertical stacking of atomically thin materials offers a large platform for realizing novel properties enabled by proximity effects and moiré patterns. Here we focus on mechanically assembled heterostructures of graphene and ReS$_2$, a van der Waals layered semiconductor. Using scanning tunneling microscopy and spectroscopy (STM/STS) we image the sharp edge between the two materials as well as areas of overlap. Locally resolved topographic images revealed the presence of a striped superpattern originating in the interlayer interactions between graphene's hexagonal structure and the triclinic, l…
Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学）；Technical University Darmstadt（达姆施塔特工业大学）；Ulm University（乌尔姆大学）；National Institute for Materials Science（国立材料研究所）
Two-dimensional materials and their van der Waals heterostructures enable a large range of applications, including label-free biosensing. Lattice mismatch and work function difference in the heterostructure material result in strain and charge transfer, often varying at nanometer scale, that influence device performance. In this work, a multidimensional optical imaging technique is developed in order to map sub-diffractional distributions for doping and strain and understand the role of those for modulation of electronic properties of the material. As an example, vertical heterostructure compr…
Vertically stacking two dimensional (2D) materials can enable the design of novel electronic and optoelectronic devices and realize complex functionality. However, the fabrication of such artificial heterostructures in wafer scale with an atomically-sharp interface poses an unprecedented challenge. Here, we demonstrate a convenient and controllable approach for the production of wafer-scale 2D GaSe thin films by molecular beam epitaxy. In-situ reflection high-energy electron diffraction oscillations and Raman spectroscopy reveal a layer-by-layer van der Waals epitaxial growth mode. Highly-effi…
Graphene/silicon heterostructures have attracted tremendous interest as a new platform for diverse electronic and photonic devices such as barristors, solar cells, optical modulators, and chemical sensors. The studies to date largely focus on junctions between graphene and lightly-doped silicon, where a Schottky barrier is believed to dominate the carrier transport process. Here we report a systematic investigation of carrier transport across the heterojunctions formed between graphene and highly-doped silicon. By varying the silicon doping level and the measurement temperature, we show that t…
Finding alternative optoelectronic mechanisms that overcome the limitations of conventional semiconductor devices is paramount for detecting and harvesting low-energy photons. A highly promising approach is to drive a current from the thermal energy added to the free-electron bath as a result of light absorption. Successful implementation of this strategy requires a broadband absorber where carriers interact among themselves more strongly than with phonons, as well as energy-selective contacts to extract the excess electronic heat. Here we show that graphene-WSe2-graphene heterostructure devic…
The celebrated electronic properties of graphene have opened way for materials just one-atom-thick to be used in the post-silicon electronic era. An important milestone was the creation of heterostructures based on graphene and other two-dimensional (2D) crystals, which can be assembled in 3D stacks with atomic layer precision. These layered structures have already led to a range of fascinating physical phenomena, and also have been used in demonstrating a prototype field effect tunnelling transistor - a candidate for post-CMOS technology. The range of possible materials which could be incorpo…
Initiating impact ionization of avalanche breakdown essentially requires applying a high electric field in a long active region, hampering carrier-multiplication with high gain, low bias and superior noise performance. Here we report the observation of ballistic avalanche phenomena in sub-MFP scaled vertical indium selenide (InSe)/black phosphorus (BP) heterostructures. The heterojunction is engineered to avalanche photodetectors (APD) and impact ionization transistors, demonstrating ultra-sensitive mid-IR light detection (4 μm wavelength) and ultra-steep subthreshold swing, respectively. Thes…
The improved photocatalytic water splitting using 2D materials has technological importance for economically viable renewable energy. The present study focuses on the effect of uniaxial, biaxial, and vertical strain on the energy gap and band edge positions of C2N/MoS2 van der Waals heterostructures through first-principles density functional theory using PBE and SCAN functionals. The calculations establish that SCAN functional provides comparatively much better results as compared to the PBE for the band gap and band alignment study. The heterostructure exhibits a type- II band alignment whic…
Atomically thin black phosphorus (BP) is a promising two-dimensional material for fabricating electronic and optoelectronic nano-devices with high mobility and tunable bandgap structures. However, the charge-carrier mobility in few-layer phosphorene (monolayer BP) is mainly limited by the presence of impurity and disorders. In this study, we demonstrate that vertical BP heterostructure devices offer great advantages in probing the electron states of monolayer and few-layer phosphorene at temperatures down to 2 K through capacitance spectroscopy. Electronic states in the conduction and valence …
Recent works have revealed that van der Waals (vdW) epitaxial growth of 2D materials on crystalline substrates, such as hexagonal boron nitride (hBN), leads to formation of self-aligned grains, which results in defect-free stitching between the grains. However, how the weak vdW interaction causes strong limitation on orientation of grains is still not understood yet. In this work, we have focused on investigation of mechanism of self-alignment of MoS2 grains in vdW epitaxial growth on hBN. Through calculation based on density functional theory and the Lennard-Jones potential, we found that int…
Vertical integration of two-dimensional van der Waals materials is predicted to lead to novel electronic and optical properties not found in the constituent layers. Here, we present the direct synthesis of two unique, atomically thin, multi-junction heterostructures by combining graphene with the monolayer transition-metal dichalocogenides: MoS2, MoSe2, and WSe2.The realization of MoS2-WSe2-Graphene and WSe2-MoSe2-Graphene heterostructures leads toresonant tunneling in an atomically thin stack with spectrally narrow room temperature negative differential resistance characteristics.
Vertical integration of two-dimensional materials has recently emerged as an exciting method for the design of novel electronic and optoelectronic devices. Using density functional theory, we investigatethe structural and electronic properties of two heterostruc-tures, graphene/phosphorene (G/BP) and hexagonal boron nitride/phosphorene (BN/BP). We found that the interlayer distance, binding energy, and charge transfer in G/BP and BN/BP are similar. Interlayer noncovalentbonding is predicted due to the weak coupling between the pz orbital of BP and the π orbital of graphene and BN. A small amou…
Semiconductor heterostructures provide a powerful platform for the engineering of excitons. Here we report the excitonic properties of two-dimensional (2D) heterostructures that consist of monolayer MoS2 and WS2 stacked epitaxially or non-epitaxially in the vertical direction. We find similarly efficient interlayer relaxation and transition of excitons in both the epitaxial and nonepitaxial heterostructures. This is manifested by a two orders of magnitude decrease in the photoluminescence and the appearance of an extra absorption peak at low energy region. The MoS2/WS2 heterostructures show we…
Graphene-based vertical heterostructures, particularly stacks incorporated with other layered materials, are promising for nanoelectronics. The stacking of two model Dirac materials, graphene and topological insulator, can considerably enlarge the family of van der Waals heterostructures. Despite well understanding of the two individual materials, the electron transport properties of a combined vertical heterojunction are still unknown. Here we show the experimental realization of a vertical heterojunction between Bi2Se3 nanoplate and monolayer graphene. At low temperatures, the electron trans…
Van der Waals heterostructures formed by stacking different atomically thin layered materials have emerged as the sought-after device platform for electronic and optoelectronic applications. Determining the spatial extent of all the encapsulated components in such vertical stacks is key to optimal fabrication methods and improved device performance. Here we employ electrostatic force microscopy as a fast and non-invasive microscopic probe that provides compelling images of two dimensional layers buried over 30 nm below the sample surface. We demonstrate the versatility of the technique by stud…
The fabrication of artificial materials by stacking of individual two-dimensional (2D) materials is amongst one of the most promising research avenues in the field of 2D materials. Moreover, this strategy to fabricate new man-made materials can be further extended by fabricating hybrid stacks between 2D materials and other functional materials with different dimensionality making the potential number of combinations almost infinite. Among all these possible combinations, mixing 2D materials with transition metal oxides can result especially useful because of the large amount of interesting phy…
It is a persisting pursuit to use metal as a channel material in a field effect transistor. All metallic transistor can be fabricated from pristine semimetallic Dirac materials (such as graphene, silicene, and germanene), but the on/off current ratio is very low. In a vertical heterostructure composed by two Dirac materials, the Dirac cones of the two materials survive the weak interlayer van der Waals interaction based on density functional theory method, and electron transport from the Dirac cone of one material to the one of the other material is therefore forbidden without assistance of ph…
We present research results on the electronic transport in heterostructures based on p-type nickel oxide (NiO) with the n-type oxide semiconductors zinc oxide (ZnO) and cadmium oxide (CdO). NiO is a desirable candidate for application in (opto-)electronic devices. However, because of its small electron affinity, heterojunctions with most n-type oxide semiconductors exhibit conduction and valence band offsets at the heterointerface in excess of 1 eV. ZnO/NiO junctions exhibit a so called type-II band alignment, making electron-hole recombination the only process by which a current can verticall…
Black phosphorus (BP) has recently emerged as a promising narrow band gap layered semiconductor with optoelectronic properties that bridge the gap between semi-metallic graphene and wide band gap transition metal dichalcogenides such as MoS2. To date, BP field-effect transistors have utilized a lateral geometry with in-plane transport dominating device characteristics. In contrast, we present here a vertical field-effect transistor geometry based on a graphene/BP van der Waals heterostructure. The resulting device characteristics include high on-state current densities (> 1600 A/cm2) and curre…
Placing graphene on SnS2 results in significant charge transfer, on the order of 10^13/cm^2, from the graphene to the SnS2, and the charge transfer results in a negative Schottky barrier contact for electron injection from the graphene into the SnS2 conduction band. However, due to the s-px,y composition of the SnS2 conduction band, the coupling between the SnS2 and the graphene is relatively weak. A third layer, HfSe2, placed between the SnS2 and the graphene, serves as a matrix element matching layer, since it has strong coupling to both the graphene and the SnS2. It increases the coupling t…
Intensive efforts have been devoted to exploit novel optoelectronic devices based on two-dimensional (2D) transition-metal dichalcogenides (TMDCs) owing to their strong light-matter interaction and distinctive material properties. In particular, photodetectors featuring both high-speed and high-responsivity performance are of great interest for a vast number of applications such as high-data-rate interconnects operated at standardized telecom wavelengths. Yet, the intrinsically small carrier mobilities of TMDCs become a bottleneck for high-speed application use. Here, we present high-performan…
Raman enhancement techniques are essential for fundamental studies in light-matter interactions and find widespread application in microelectronics, bio-chemical sensing, and clinical diagnosis. Two-dimensional (2D) materials and their van der Waals heterostructures (vdWHs) are emerging rapidly as potential platforms for Raman enhancement. Here, we experimentally demonstrate a new technique of Raman enhancement driven by nonradiative energy transfer (NRET) achieving a $10$-fold enhancement in the Raman intensity in a vertical vdWH comprising of a monolayer transition metal dichalcogenide (1L-T…
We investigate a two-dimensional (2D) heterostructure consisting of few-layer direct bandgap ReS2, a thin h-BN layer and a monolayer graphene for application to various electronic devices. Metal-insulator-semiconductor (MIS)-type devices with two-dimensional (2D) van-der-Waals (vdW) heterostructures have recently been studied as important components to realize various multifunctional device applications in analogue and digital electronics. The tunnel diodes of ReS2/h-BN/graphene exhibit light tuneable rectifying behaviours with low ideality factors and nearly temperature independent electrical…
We investigate interlayer tunneling in heterostructures consisting of two tungsten diselenide (WSe2) monolayers with controlled rotational alignment, and separated by hexagonal boron nitride. In samples where the two WSe2 monolayers are rotationally aligned we observe resonant tunneling, manifested by a large conductance and negative differential resistance in the vicinity of zero interlayer bias, which stem from energy- and momentum-conserving tunneling. Because the spin-orbit coupling leads to coupled spin-valley degrees of freedom, the twist between the two WSe2 monolayers allows us to prob…
We identify a new universality in the carrier transport of two-dimensional(2D)-material-based Schottky heterostructures. We show that the reversed saturation current ($\mathcal{J}$) scales universally with temperature ($T$) as $ \log(\mathcal{J}/T^β) \propto -1/T$, with $β= 3/2$ for lateral Schottky heterostructures and $β= 1$ for vertical Schottky heterostructures, over a wide range of 2D systems including nonrelativistic electron gas, Rashba spintronic system, single and few-layer graphene, transition metal dichalcogenides and thin-films of topological solids. Such universalities originate f…
The vertical stacking of van der Waals (vdW) materials introduces a new degree of freedom to the research of two-dimensional (2D) systems. The interlayer coupling strongly influences the band structure of the heterostructures, resulting in novel properties that can be utilized for electronic and optoelectronic applications. Based on microwave microscopy studies, we report quantitative electrical imaging on gated molybdenum disulfide (MoS2)/tungsten diselenide (WSe2) heterostructure devices, which exhibit an intriguing anti-ambipolar effect in the transfer characteristics. Interestingly, in the…
Bilayer van der Waals (vdW) heterostructures such as MoS2/WS2 and MoSe2/WSe2 have attracted much attention recently, particularly because of their type II band alignments and the formation of interlayer exciton as the lowest-energy excitonic state. In this work, we calculate the electronic and optical properties of such heterostructures with the first-principles GW+Bethe-Salpeter Equation (BSE) method and reveal the important role of interlayer coupling in deciding the excited-state properties, including the band alignment and excitonic properties. Our calculation shows that due to the interla…
Vertical and lateral heterostructures of van der Waals materials provide tremendous flexibility for band structure engineering. Since electronic bands are sensitively affected by defects, strain, and interlayer coupling, the edge and heterojunction of these two-dimensional (2D) systems may exhibit novel physical properties, which can be fully revealed only by spatially resolved probes. Here, we report the spatial mapping of photoconductivity in a monolayer-bilayer WSe2 lateral heterostructure under multiple excitation lasers. As the photon energy increases, the light-induced conductivity detec…
Light emission in atomically thin heterostructures is known to depend on the type of materials, number and stacking sequence of the constituent layers. Here we show that the thickness of a two-dimensional substrate can be crucial in modulating the light emission. We study the layer-dependent charge transfer in vertical heterostructures built from monolayer tungsten disulphide (WS2) on one- and two-layer epitaxial graphene, unravelling the effect that the interlayer electronic coupling has on the excitonic properties of such heterostructures. We bring evidence that the excitonic properties of W…
Combining both vertical and in-plane two-dimensional (2D) heterostructures opens up the possibility to create an unprecedented architecture using 2D atomic layer building blocks. The thermal transport properties of such mixed heterostructures, critical to various applications in nanoelectronics, however, have not been thoroughly explored. Herein, we construct two configurations of multilayer in-plane graphene/hexagonal boron nitride (Gr/h-BN) heterostructures (i.e. mixed heterostructures) via weak van der Waals (vdW) interactions and systematically investigate the dependence of their interfaci…
The discovery of Berry curvature (BC) has spurred a tremendous surge of research into various quantum phenomena such as the anomalous transport of electrons and the topological phases of matter. In two-dimensional crystalline systems, the conventional definition of the BC lacks the in-plane components and thus it cannot explain the transverse transport along the plane-normal direction. Here, we modify the BC to newly provide in-plane components in two dimensions, giving rise to the vertical Hall effects that describe out-of-plane transports in response to in-plane perturbations and their Onsag…
Vertically stacked van der Waals heterostructures are a lucrative platform for exploring the rich electronic and optoelectronic phenomena in two-dimensional materials. Their performance will be strongly affected by impurities and defects at the interfaces. Here we present the first systematic study of interfaces in van der Waals heterostructure using cross sectional scanning transmission electron microscope (STEM) imaging. By measuring interlayer separations and comparing these to density functional theory (DFT) calculations we find that pristine interfaces exist between hBN and MoS2 or WS2 fo…
