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 studying heterojunctions comprising graphene, hexagonal boron nitride and transition metal dichalcogenides. Work function of each constituent layer acts as a unique fingerprint during imaging, thereby providing important insights into the charge environment, disorder, structural imperfections and doping profile. The technique holds great potential for gaining a comprehensive understanding of the quality, flatness as well as local electrical properties of buried layers in a large class of nanoscale materials and vertical heterostructures.
We report experimental and computational studies of thermal transport properties in hexagonal boron nitride (hBN) encapsulated molybdenum disulfide (MoS2) structure using refined optothermal Raman techniques, and reveal very high interfacial thermal conductance between hBN and MoS2. By studying the Raman shift of hBN and MoS2 in suspended and substrate-supported thin films under varying laser power and temperature, we calibrate lateral (in-plane) thermal conductivity of hBN and MoS2 and the vertical interfacial thermal conductance in the hBN/MoS2/hBN heterostructure as well as the interfaces b…
Quantum spin-liquid van der Waals magnets such as TaS$_2$, TaSe$_2$, and RuCl$_3$ provide a natural platform to explore new exotic phenomena associated with spinon physics, whose properties can be controlled by exchange proximity with ferromagnetic insulators such as CrBr$_3$. Here we put forward a twisted van der Waals heterostructure based on a quantum spin-liquid bilayer encapsulated between ferromagnetic insulators. We demonstrate the emergence of spinon flat bands and topological spinon states in such heterostructure, where the emergence of a topological gap is driven by the twist. We fur…
We investigate the geometry, stability, electronic structure and optical properties of C24H12 coronenes encapsulated in a single-wall (19,0) carbon nanotube. By an adequate combination of advanced electronic-structure techniques, involving weak and van derWaals interaction, as well as many-body effects for establishing electronic properties and excitations, we have accurately characterized this hybrid carbon nanostructure, which arises as a promising candidate for opto-electronic nanodevices. In particular, we show that the structure of the stacked coronenes inside the nanotube is characterize…
Twisted van der Waals materials have become a paradigmatic platform to realize exotic correlated states of matter. Here, we show that a twisted dichalcogenide bilayer (WSe$_2$) encapsulated between a magnetic van der Waals material (CrBr$_3$) features flat bands with tunable valley and spin flavors. We demonstrate that, when electron-electron interactions are included, spin-ferromagnetic and valley-ferromagnetic states emerge in the flat bands, stemming from the interplay between correlations, intrinsic spin-orbit coupling and exchange proximity effects. We show that the specific symmetry brok…
Tellurium can form nanowires of helical atomic chains. Given their unique one-dimensional van der Waals structure, these nanowires are expected to show remarkably different physical and electronic properties than bulk tellurium. Here we show that few-chain and single-chain van der Waals tellurium nanowires can be isolated using carbon nanotube and boron nitride nanotube encapsulation. With the approach, the number of atomic chains can be controlled by the inner diameter of the nanotube. The Raman response of the structures suggests that the interaction between a single-atomic tellurium chain a…
High-temperature cuprate superconductors-based van der Waals (vdW) heterostructures hold high technological promise. One of the obstacles hindering progress is the detrimental effect of disorder on the properties of Josephson junctions (JJ) realized by the vdW devices. Here we report the new method of fabricating twisted vdW heterostructures made of Bi2Sr2CuCa2O8+d, crucially improving the JJ characteristics, pushing them up to those of the intrinsic JJs in bulk samples. The method combines a cryogenic stacking using a solvent-free stencil mask technique and covering interface by the insulatin…
Accessing intrinsic properties of a graphene device can be hindered by the influence of contact electrodes. Here, we capacitively couple graphene devices to superconducting resonant circuits and observe clear changes in the resonance- frequency and -widths originating from the internal charge dynamics of graphene. This allows us to extract the density of states and charge relaxation resistance in graphene p-n junctions without the need of electrical contacts. The presented characterizations pave a fast, sensitive and non-invasive measurement of graphene nanocircuits.
Van der Waals heterostructures provide a rich platform for emergent physics due to their tunable hybridization of electronic orbital- and spin-degrees of freedom. Here, we show that a heterostructure formed by twisted bilayer graphene sandwiched between ferromagnetic insulators develops flat bands stemming from the interplay between twist, exchange proximity and spin-orbit coupling. We demonstrate that in this flat-band regime, the spin degree of freedom is hybridized, giving rise to an effective triangular superlattice with valley as a degenerate pseudospin degree of freedom. Incorporating el…
The assembly of individual two-dimensional materials into van der Waals heterostructures enables the construction of layered three-dimensional materials with desirable electronic and optical properties. A core problem in the fabrication of these structures is the formation of clean interfaces between the individual two-dimensional materials which would affect device performance. We present here a technique for the rapid batch fabrication of van der Waals heterostructures, demonstrated by the controlled production of 22 mono-, bi- and trilayer graphene stacks encapsulated in hexagonal boron nit…
Opto-electronic devices utilizing graphene have already demonstrated unique capabilities, which are much more difficult to realize with conventional technologies. However, the requirements in terms of material quality and uniformity are very demanding. A major roadblock towards high-performance devices are the nanoscale variations of graphene properties, which strongly impact the macroscopic device behaviour. Here, we present and apply opto-electronic nanoscopy to measure locally both the optical and electronic properties of graphene devices. This is achieved by combining scanning near-field i…
Establishing ohmic contact to van der Waals semiconductors such as MoS2 is crucial to unlocking their full potential in next-generation electronic devices. Encapsulation of few layer MoS2 with hBN preserves the material's electronic properties but makes electrical contacts more challenging. Progress toward high quality edge contact to encapsulated MoS2 has been recently reported. Here, we evaluate a contact methodology using sputtered MoRe, a Type II superconductor with a relatively high critical field and temperature commonly used to induce superconductivity in graphene. We find that the cont…
We have combined spatially-resolved steady-state micro-photoluminescence ($μ$PL) with time-resolved photoluminescence (TRPL) to investigate the exciton diffusion in a WSe$_2$ monolayer encapsulated with hexagonal boron nitride (hBN). At 300 K, we extract an exciton diffusion length $L_X= 0.36\pm 0.02 \; μ$m and an exciton diffusion coefficient of $D_X=14.5 \pm 2\;\mbox{cm}^2$/s. This represents a nearly 10-fold increase in the effective mobility of excitons with respect to several previously reported values on nonencapsulated samples. At cryogenic temperatures, the high optical quality of thes…
The presence of finite bandgap and high mobility in semiconductor few-layer black phosphorus offers an attractive prospect for using this material in future two-dimensional electronic devices. Here we demonstrate for the first time fully encapsulated ultrathin (down to bilayer) black phosphorus field effect transistors in Van der Waals heterostructures to preclude their stability and degradation problems which have limited their potential for applications. Introducing monolayer graphene in our device architecture for one-atom-thick conformal source-drain electrodes enables a chemically inert b…
We propose a spin valve that is based on van der Waals antiferromagnetism and fully electrically controlled. The device is composed of two antiferromagnetic terminals that allow for vertical bias control and a linked central scattering potential region. The magnetoresistance varies significantly when the bias orientations in two terminals are switched from parallel to antiparallel because this switch induces a mismatch of the bands for the same spin projection in different parts of the system. It is shown from density functional calculations that bilayer graphene encapsulated by two atomic lay…
The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of …
Ferroelectric van der Waals heterostructures provide a natural platform to design a variety of electrically controllable devices. In this work, we demonstrate that AB bilayer graphene encapsulated in MoTe$_2$ acts as a valley valve that displays a switchable built-in topological gap, leading to ferroelectrically driven topological channels. Using a combination of ab initio calculations and low energy models, we show that the ferroelectric order of MoTe$_2$ allows the control of the gap opening in bilayer graphene and leads to topological channels between different ferroelectric domains. Moreov…
Raman scattering is a ubiquitous phenomenon in light-matter interactions which reveals a material's electronic, structural and thermal properties. Controlling this process would enable new ways of studying and manipulating fundamental material properties. Here, we report a novel Raman scattering process at the interface between different van der Waals (vdW) materials as well as between a monolayer semiconductor and 3D crystalline substrates. We find that interfacing a WSe2 monolayer with materials such as SiO2, sapphire, and hexagonal boron nitride (hBN) enables Raman transitions with phonons …
We have realized encapsulated trilayer MoS$_2$ devices with gated graphene contacts. In the bulk, we observe an electron mobility as high as 7000~cm$^{2}$/(V s) at a density of 3 $\times$ 10$^{12}$~cm$^{-2}$ at a temperature of 1.9~K. Shubnikov--de Haas oscillations start at magnetic fields as low as 0.9~T. The observed 3-fold Landau level degeneracy can be understood based on the valley Zeeman effect. Negatively biased split gate electrodes allow us to form a channel that can be completely pinched off for sufficiently large gate voltages. The measured conductance displays plateau-like feature…
Atomically transparent vertically aligned ZnO-based van der Waals material have been developed by surface passivation and encapsulation with atomic layers of MgO using materials by design; the physical properties investigated. The passivation and encapsulation led to a remarkable improvement in optical and electronic properties. The valence-band offset $ΔE_v$ between MgO and ZnO, ZnO and MgO/ZnO, and ZnO and MgO/ZnO/MgO heterointerfaces are determined to be 0.37 $\pm$0.02, -0.05$\pm$0.02, and -0.11$\pm$0.02 eV, respectively; the conduction-band offset $ΔE_c$ is deduced to be 0.97$\pm$0.02, 0.4…
Vertically stacked van der Waals heterostructures are a lucrative platform for exploring the rich electronic and optoelectronic phenomena in two-dimensional materials. Their performance will be strongly affected by impurities and defects at the interfaces. Here we present the first systematic study of interfaces in van der Waals heterostructure using cross sectional scanning transmission electron microscope (STEM) imaging. By measuring interlayer separations and comparing these to density functional theory (DFT) calculations we find that pristine interfaces exist between hBN and MoS2 or WS2 fo…
Designer heterostructures can now be assembled layer-by-layer with unmatched precision thanks to the recently developed deterministic placement methods to transfer two-dimensional (2D) materials. This possibility constitutes the birth of a very active research field on the so-called van der Waals heterostructures. Moreover, these deterministic placement methods also open the door to fabricate complex devices, which would be otherwise very difficult to achieve by conventional bottom-up nanofabrication approaches, and to fabricate fully-encapsulated devices with exquisite electronic properties. …
Heterostructures formed between two different van der Waals materials enable interactions and functionalities absent in each component. In this work we show that vicinity to an atomically thin WSe$_2$ sheet dramatically impacts the energies of the symmetry-broken low Landau levels of bilayer graphene, possibly due to screening. We present a systematic study of the magnetic field and electrical displacement field dependences of the Landau level gaps at filling factor $ν$ = 1, 2, 3, and compare to BN encapsulated pristine bilayer graphene. The exchange-dominated energy splitting between the N = …
We have fabricated an encapsulated monolayer MoS$_{\mathrm{2}}$ device with metallic ohmic contacts through a pre-patterned hBN layer. In the bulk, we observe an electron mobility as high as 3000 cm$^{\mathrm{2}}$/Vs at a density of 7 $\times$ 10$^{\mathrm{12}}$ cm$^{\mathrm{-2}}$ at a temperature of 1.7 K. Shubnikov-de Haas oscillations start at magnetic fields as low as 3.3 T. By realizing a single quantum dot gate structure on top of the hBN we are able to confine electrons in MoS$_{\mathrm{2}}$ and observe the Coulomb blockade effect. By tuning the middle gate voltage we reach a double dot…
Two dimensional materials are usually envisioned as flat, truly 2D layers. However out-of-plane corrugations are inevitably present in these materials. In this manuscript, we show that graphene flakes encapsulated between insulating crystals (hBN, WSe2), although having large mobilities, surprisingly contain out-of-plane corrugations. The height fluctuations of these corrugations are revealed using weak localization measurements in the presence of a static in-plane magnetic field. Due to the random out-of-plane corrugations, the in-plane magnetic field results in a random out-of-plane componen…
We report the observation of optical second harmonic generation (SHG) in single-layer indium selenide (InSe). We measure a second harmonic signal of $>10^3$ $\textrm{cts/s}$ under nonresonant excitation using a home-built confocal microscope and a standard pulsed pico-second laser. We demonstrate that polarization-resolved SHG serves as a fast, non-invasive tool to determine the crystal axes in single-layer InSe and to relate the sharp edges of the flake to the armchair and zigzag edges of the crystal structure. Our experiment determines these angles to an accuracy better than $\pm$ $0.2^{\cir…
We propose a robust and efficient way of controlling the optical spectra of two-dimensional materials and van der Waals heterostructures by quantum cavity embedding. The cavity light-matter coupling leads to the formation of exciton-polaritons, a superposition of photons and excitons. Our first principles study demonstrates a reordering and mixing of bright and dark excitons spectral features and in the case of a type II van-der-Waals heterostructure an inversion of intra and interlayer excitonic resonances. We further show that the cavity light-matter coupling strongly depends on the dielectr…
Van der Waals heterostructures constitute a platform for investigating intriguing many-body quantum phenomena. In particular, transition-metal dichalcogenide (TMD) hetero-bilayers host long-lived interlayer excitons which exhibit permanent out-of-plane dipole moments. Here, we develop a microscopic theory for interlayer exciton-exciton interactions including both the dipolar nature of interlayer excitons as well as their fermionic substructure, which gives rise to an attractive fermionic exchange. We find that these interactions contribute to a drift force resulting in highly non-linear excito…
The Raman 2D line of graphene is widely used for device characterization and during device fabrication as it contains valuable information on e.g. the direction and magnitude of mechanical strain and doping. Here we present systematic asymmetries in the 2D line shape of exfoliated graphene and graphene grown by chemical vapor deposition. Both graphene crystals are fully encapsulated in van der Waals heterostructures, where hexagonal boron nitride and tungsten diselenide are used as substrate materials. In both material stacks, we find very low doping values and extremely homogeneous strain dis…
Two-dimensional (2D) transition metal dichalcogenides (TMDCs) are the subject of intense investigation for applications in optics, electronics, catalysis, and energy storage. Their optical and electronic properties can be significantly enhanced when encapsulated in an environment that is free of charge disorder. Because hexagonal boron nitride (h-BN) is atomically thin, highly-crystalline, and is a strong insulator, it is one of the most commonly used 2D materials to encapsulate and passivate TMDCs. In this report, we examine how ultrathin h-BN shields an underlying MoS2 TMDC layer from the en…
We investigate the proximity spin-orbit and exchange couplings in ABA and ABC trilayer graphene encapsulated within monolayers of semiconducting transition-metal dichalcogenides and the ferromagnetic semiconductor Cr$_2$Ge$_2$Te$_6$. Employing first-principles calculations we obtain the electronic structures of the multilayer stacks and extract the relevant proximity-induced orbital and spin interaction parameters by fitting the low-energy bands to model Hamiltonians. We also demonstrate the tunability of the proximity effects by a transverse electric field. Using the model Hamiltonians we als…
The recently observed unconventional ferroelectricity in AB bilayer graphene sandwiched by hexagonal Boron Nitride (hBN) presents a new platform to manipulate correlated phases in multilayered van der Waals heterostructures. We present a low-energy continuum model for AB bilayer graphene encapsulated by the top and bottom layers of either hBN or graphene, with two independent twist angles. For the graphene/hBN heterostructures, we show that twist angle asymmetry leads to a layer polarization of the valence and conduction bands. We also show that an out-of-plane displacement field not only tune…
The optical and electronic properties of van der Waals (vdW) heterostructures depend strongly on the atomic stacking order of the constituent layers. This is exemplified by periodic variation of the local atomic registry, known as moire patterns, giving rise to superconductivity and ferromagnetism in twisted bilayer graphene and novel exciton states in transition metal dichalcogenides (TMD) heterobilayers. However, the presence of the nanometer-scale moire superlattices is typically deduced indirectly, because conventional imaging techniques, such as transmission electron microscopy (TEM), req…
Due to the chemical inertness of 2D hexagonal-Boron Nitride (h-BN), few atomic-layer h-BN is often used to encapsulate air-sensitive 2D crystals such as Black Phosphorus (BP). However, the effects of h-BN on Schottky barrier height, doping and contact resistance are not well known. Here, we investigate these effects by fabricating h-BN encapsulated BP transistors with cobalt (Co) contacts. In sharp contrast to directly Co contacted p-type BP devices, we observe strong n-type conduction upon insertion of the h-BN at the Co/BP interface. First principles calculations show that this difference ar…
Atomically thin two-dimensional (2D) semiconductors such as molybdenum disulphide (MoS2) hold great promise in electrical, optical, and mechanical devices and display novel physical phenomena such as coupled spin-valley physics and the valley Hall effect. However, the electron mobility of mono- and few-layer MoS2 has so far been substantially below theoretically predicted limits, particularly at low temperature (T), which has hampered efforts to observe its intrinsic quantum transport behaviors. Potential sources of disorder and scattering include both defects such as sulfur vacancies in the M…
Like silicon-based semiconductor devices, van der Waals heterostructures will require integration with high-K oxides. This is needed to achieve suitable voltage scaling, improved performance as well as allowing for added functionalities. Unfortunately, commonly used high-k oxide deposition methods are not directly compatible with 2D materials. Here we demonstrate a method to embed a multi-functional few nm thick high-k oxide within van der Waals devices without degrading the properties of the neighbouring 2D materials. This is achieved by in-situ laser oxidation of embedded few layer HfS2 crys…
Direct Nanoscale Pyroelectric Characterization of a CuInP${}_2$S${}_6$ van der Waals Nanogenerator
Université catholique de Louvain (UCLouvain)（天主教鲁汶大学）；Lancaster University（兰卡斯特大学）；University of Chemistry and Technology Prague（布拉格化工大学）；University of Glasgow（格拉斯哥大学）；WEL Research Institute（WEL研究所）
Van der Waals (vdW) heterostructures consisting of bilayer graphene (BLG) encapsulated within monolayers of strong spin-orbit semiconductor WS$_2$ or ferromagnetic semiconductor Cr$_2$Ge$_2$Te$_6$ (CGT), are investigated. By performing realistic first-principles calculations we capture the essential BLG band structure features, including layer- and sublattice-resolved proximity spin-orbit or exchange couplings. For different relative twist angles (0 or 60$^{\circ}$) of the WS$_2$ layers, and the magnetizations (parallel or antiparallel) of the CGT layers, with respect to BLG, the low energy ba…
By stacking various two-dimensional (2D) atomic crystals [1] on top of each other, it is possible to create multilayer heterostructures and devices with designed electronic properties [2-5]. However, various adsorbates become trapped between layers during their assembly, and this not only affects the resulting quality but also prevents the formation of a true artificial layered crystal upheld by van der Waals interaction, creating instead a laminate glued together by contamination. Transmission electron microscopy (TEM) has shown that graphene and boron nitride monolayers, the two best charact…
We present a device scheme to explore mesoscopic transport through molybdenum disulfide (MoS$_2$) constrictions using photodoping. The devices are based on van-der-Waals heterostructures where few-layer MoS$_2$ flakes are partially encapsulated by hexagonal boron nitride (hBN) and covered by a few-layer graphene flake to fabricate electrical contacts. Since the as-fabricated devices are insulating at low temperatures, we use photo-induced remote doping in the hBN substrate to create free charge carriers in the MoS$_2$ layer. On top of the device, we place additional metal structures, which def…
The dry release transfer of two-dimensional (2D) materials such as graphene, h-BN, and TMDs is a versatile method for fabricating high-quality van der Waals heterostructures. Up until now, polydimethylpolysiloxane (PDMS) sheets have been widely used for the dry release transfer of TMD materials. However, this method has been known to have limitations that make it difficult to transfer few-layer-thick graphene and h-BN because of the difficulty to fabricate these materials on PDMS. As an alternative method, we demonstrate the dry release transfer of single- and bi-layer graphene and few-layer h…
