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Two-dimensional (2D) moire materials provide a new solid-state platform with unprecedented controllability for studies of correlated quantum phenomena. To date, experimental studies have focused on the correlated electronic states; the correlated bosonic states in moire materials have remained practically unexplored. Here, we report a correlated dipolar excitonic insulator, a charge insulating state driven by the formation of excitons, in a Coulomb-coupled WSe2 monolayer and WSe2/WS2 moire bilayer at total hole doping density equal to the moire density. The system is a Mott insulator when all the holes reside in the moire layer. Under an out-of-plane electric field, the holes can be continuously transferred to the WSe2 monolayer, but remain strongly bound to the empty moire sites; they form an interlayer exciton fluid in the moire superlattice under a particle-hole transformation. We identify the phase space and determine the charge gap energy of the excitonic insulating state by optical spectroscopy and capacitance measurements, respectively. We further observe the emergence of local magnetic moments in the WSe2 monolayer induced by the strong interlayer Coulomb correlation. Our demonstration of an exciton fluid in a lattice paves the path for realizing correlated bosonic quantum phenomena described by the Bose-Hubbard model in a solid-state system.

Heterostructures made from van der Waals materials provide a template to investigate proximity effects at atomically sharp heterointerfaces. In particular, near-field charge and energy transfer in heterostructures made from semiconducting transition metal dichalcogenides (TMD) have attracted interest to design model 2D "donor-acceptor" systems and new optoelectronic components. Here, using of Raman scattering and photoluminescence spectroscopies, we report a comprehensive characterization of a molybedenum diselenide (MoSe$_2$) monolayer deposited onto hexagonal boron nitride (hBN) and capped by mono- and bilayer graphene. Along with the atomically flat hBN susbstrate, a single graphene epilayer is sufficient to passivate the MoSe$_2$ layer and provides a homogenous environment without the need for an extra capping layer. As a result, we do not observe photo-induced doping in our heterostructure and the MoSe$_2$ excitonic linewidth gets as narrow as 1.6~meV, hence approaching the homogeneous limit. The semi-metallic graphene layer neutralizes the 2D semiconductor and enables picosecond non-radiative energy transfer that quenches radiative recombination from long-lived states. Hence, emission from the neutral band edge exciton largely dominates the photoluminescence spectrum of the MoSe$_2$/graphene heterostructure. Since this exciton has a picosecond radiative lifetime at low temperature, comparable with the energy transfer time, its low-temperature photoluminescence is only quenched by a factor of $3.3 \pm 1$ and $4.4 \pm 1$ in the presence of mono- and bilayer graphene, respectively. Finally, while our bare MoSe$_2$ on hBN exhibits negligible valley polarization at low temperature and under near-resonant excitation, we show that interfacing MoSe$_2$ with graphene yields a single-line emitter with degrees of valley polarization and coherence up to $\sim 15\,\%$., version 3, 5 figures

Monolayer molybdenum di-selenide (1L-MoSe2) stands out in the transition metal dichalcogenide family of materials as an outlier where optical generation of valley polarization is inefficient. Here we show that using charge doping in conjunction with an external magnetic field, the valley polarization of 1L-MoSe2 can be controlled effectively. Most remarkably, the valley polarization can be tuned to negative values, where the higher energy Zeeman mode emission is more intense than the lower energy one. Our experimental observations are interpreted with valley-selective exciton-charge dressing that manifests when gate induced doping populates predominantly one valley in the presence of Zeeman splitting.

Moire engineering1–3 of van der Waals magnetic materials4–9 can yield new magnetic ground states via competing interactions in moire superlattices10–13. Theory predicts a suite of interesting phenomena, including multiflavour magnetic states10, non-collinear magnetic states10–13, moire magnon bands and magnon networks14 in twisted bilayer magnetic crystals, but so far such non-trivial magnetic ground states have not emerged experimentally. Here, by utilizing the stacking-dependent interlayer exchange interactions in two-dimensional magnetic materials15–18, we demonstrate a coexisting ferromagnetic (FM) and antiferromagnetic (AF) ground state in small-twist-angle CrI3 bilayers. The FM–AF state transitions to a collinear FM ground state above a critical twist angle of about 3°. The coexisting FM and AF domains result from a competition between the interlayer AF coupling, which emerges in the monoclinic stacking regions of the moire superlattice, and the energy cost for forming FM–AF domain walls. Our observations are consistent with the emergence of a non-collinear magnetic ground state with FM and AF domains on the moire length scale10–13. We further employ the doping dependence of the interlayer AF interaction to control the FM–AF state by electrically gating a bilayer sample. These experiments highlight the potential to create complex magnetic ground states in twisted bilayer magnetic crystals, and may find application in future gate-voltage-controllable high-density magnetic memory storage. In moire superlattice van der Waals magnetic materials, competing interactions emerge and can stabilize new magnetic states. Here, stacking-dependent interlayer exchange interactions in small-twist-angle CrI3 bilayers yield an ordered ground state with coexisting ferromagnetic and antiferromagnetic regions.

We have developed a simple and straightforward way to realize controlled postdoping toward 2D transition metal dichalcogenides (TMDs). The key idea is to use low-kinetic-energy dopant beams and a high-flux chalcogen beam simultaneously, leading to substitutional doping with controlled dopant densities. Atomic-resolution transmission electron microscopy has revealed that dopant atoms injected toward TMDs are incorporated substitutionally into the hexagonal framework of TMDs. The electronic properties of doped TMDs (Nb-doped WSe2) have shown drastic change and p-type action with more than 2 orders of magnitude increase in current. Position-selective doping has also been demonstrated by the postdoping toward TMDs with a patterned mask on the surface. The postdoping method developed in this work can be a versatile tool for 2D-based next-generation electronics in the future.

Phonon polaritons (PhPs) enable a variety of applications, yet it requires PhPs supported in the desired frequency range. The two BN allotropes (cubic and hexagonal, cBN and hBN) are of particular interest, as their optic phonons fall within the so-called molecular-fingerprint region (~ 1000–1610 cm−1). However, there remains a spectral gap between PhPs covered by these two, limiting applications. Thus, we isotopically engineered hBN and cBN and examined the optic phonons. For hBN, enhancement of the optic phonon lifetimes and shifted frequencies are observed. However, lifetimes are observed to decrease with the enrichment of cBN by 10B, 11B, and 15N. We propose that the reduced lifetimes are not due to intrinsic loss, but rather increased defect concentrations resulting from the modified growth, supported by first-principles calculations. Thus, reducing the extrinsic defects in isotopically engineered cBN may present a path toward overcoming these restrictions for applications in the molecular-fingerprint region.

Semiconducting monolayers of transition-metal dichalcogenides are outstanding platforms to study both electronic and phononic interactions as well as intra- and intervalley excitons and trions. The...

Gate-controlled supercurrent (GCS) in superconducting nanobridges has recently attracted attention as a means to create superconducting switches. Despite the clear advantages for applications, the microscopic mechanism of this effect is still under debate. In this work, we realize GCS for the first time in a highly crystalline superconductor epitaxially grown on an InAs nanowire. We show that the supercurrent in the epitaxial Al layer can be switched to the normal state by applying similar to +/- 23 V on a bottom gate insulated from the nanowire by a crystalline hBN layer. Our extensive study of the temperature and magnetic field dependencies suggests that the electric field is unlikely to be the origin of GCS in our device. Though hot electron injection alone cannot explain our experimental findings, a very recent non-equilibrium phonons based picture is compatible with most of our results.

Active polarization control is highly desirable in photonic systems but has been limited mostly to discrete structures in bulky dielectric media and liquid crystal–based variable retarders. Here, we report electrically reconfigurable polarization conversion across telecommunication wavelengths (1410 to 1575 nanometers) in van der Waals layered materials using tri-layer black phosphorus (TLBP) integrated in a Fabry-Pérot cavity. The large electrical tunability of birefringence in TLBP enables spectrally broadband polarization control. We found that polarization states could be generated over a large fraction of the Poincaré sphere through spectral tuning, and that electrical tuning enables the state of polarization conversion to span nearly half the Poincaré sphere. We observed both linear to circular and cross-polarization conversion with voltage, demonstrating versatility with a high dynamic range.

Doped graphene could be of use in next-generation electronic and photonic devices. However, chemical doping cannot be precisely controlled in the material and leads to external disorder that diminishes carrier mobility and conductivity. Here we show that graphene can be efficiently doped using a monolayer of tungsten oxyselenide (TOS) that is created by oxidizing a monolayer of tungsten diselenide. When the TOS monolayer is in direct contact with graphene, a room-temperature mobility of 2,000 cm2 V−1 s−1 at a hole density of 3 × 1013 cm−2 is achieved. Hole density and mobility can also be controlled by inserting tungsten diselenide interlayers between TOS and graphene, where increasing the layers reduces the disorder. With four layers, a mobility value of around 24,000 cm2 V−1 s−1 is observed, approaching the limit set by acoustic phonon scattering, resulting in a sheet resistance below 50 Ω sq−1. To illustrate the potential of our approach, we show that TOS-doped graphene can be used as a transparent conductor in a near-infrared (1,550 nm) silicon nitride photonic waveguide and ring resonator. A monolayer of tungsten oxyselenide, created by oxidizing a layer of tungsten diselenide, can be used to efficiently dope graphene, leading to a room-temperature mobility of 2,000 cm2 V–1 s–1 at a hole density of 3 × 1013 cm–2.

Moire superlattices in van der Waals (vdW) heterostructures form by stacking atomically thin layers on top of one another with a twist angle or lattice mismatch. The resulting moire potential leads to a strong modification of the band structure, which can give rise to exotic quantum phenomena ranging from correlated insulators and superconductors to moire excitons and Wigner crystals. Here, we demonstrate the dynamic tuning of moire potential in a WSe2/WS2 heterostructure at cryogenic temperature. We utilize the optical fiber tip of a cryogenic scanning near-field optical microscope (SNOM) to locally deform the heterostructure and measure its near-field optical response simultaneously. The deformation of the heterostructure increases the moire potential, which leads to a red shift of the moire exciton resonances. We observe the interlayer exciton resonance shifts up to 20 meV, while the intralayer exciton resonances shift up to 17 meV.

The spatial arrangement of adsorbates deposited onto a clean surface in vacuum typically cannot be reversibly tuned. Here we use scanning tunneling microscopy to demonstrate that molecules deposited onto graphene field-effect transistors exhibit reversible, electrically-tunable surface concentration. Continuous gate-tunable control over the surface concentration of charged F4TCNQ molecules was achieved on a graphene FET at T = 4.5K. This capability enables precisely controlled impurity doping of graphene devices and also provides a new method for determining molecular energy level alignment based on the gate-dependence of molecular concentration. The gate-tunable molecular concentration can be explained by a dynamical molecular rearrangement process that reduces total electronic energy by maintaining Fermi level pinning in the device substrate. Molecular surface concentration in this case is fully determined by the device back-gate voltage, its geometric capacitance, and the energy difference between the graphene Dirac point and the molecular LUMO level.

Heterostructure devices based on two-dimensional materials have been under intensive study due to their intriguing electrical and optical properties. One key factor in understanding these devices is their nanometer-scale band profiles, which is challenging to obtain in devices. Here, we use a technique named contact-mode scanning tunneling spectroscopy to directly visualize the band profiles of MoS2/WSe2 heterostructure devices at different gate voltages with nanometer resolution. The long-held view of a conventional p-n junction in the MoS2/WSe2 heterostructure is reexamined. Due to strong inter- and intralayer charge transfer, the MoS2 layer in contact with WSe2 is found to convert from n-type to p-type, and a series of gate-tunable p-n and p-p+ junctions are developed in the devices. Highly conductive edges are also discovered which could strongly affect the device properties.

The Wigner crystal1 has fascinated condensed matter physicists for nearly 90 years2–14. Signatures of two-dimensional (2D) Wigner crystals were first observed in 2D electron gases under high magnetic field2–4, and recently reported in transition metal dichalcogenide moire superlattices6–9. Direct observation of the 2D Wigner crystal lattice in real space, however, has remained an outstanding challenge. Conventional scanning tunnelling microscopy (STM) has sufficient spatial resolution but induces perturbations that can potentially alter this fragile state. Here we demonstrate real-space imaging of 2D Wigner crystals in WSe2/WS2 moire heterostructures using a specially designed non-invasive STM spectroscopy technique. This employs a graphene sensing layer held close to the WSe2/WS2 moire superlattice. Local STM tunnel current into the graphene layer is modulated by the underlying Wigner crystal electron lattice in the WSe2/WS2 heterostructure. Different Wigner crystal lattice configurations at fractional electron fillings of n = 1/3, 1/2 and 2/3, where n is the electron number per site, are directly visualized. The n = 1/3 and n = 2/3 Wigner crystals exhibit triangular and honeycomb lattices, respectively, to minimize nearest-neighbour occupations. The n = 1/2 state spontaneously breaks the original C3 symmetry and forms a stripe phase. Our study lays a solid foundation for understanding Wigner crystal states in WSe2/WS2 moire heterostructures and provides an approach that is generally applicable for imaging novel correlated electron lattices in other systems. So far, only indirect evidence of Wigner crystals has been reported, but a specially designed scanning tunnelling microscope is used here to directly image them in a moire heterostructure.

We report on magnetotransport in a high-quality graphene device, which is based on monolayer graphene (Gr) encapsulated by hexagonal boron nitride (hBN) layers, i.e., hBN/Gr/hBN stacks. In the vicinity of the Dirac point, a negative magnetoconductance is observed for high temperatures > ~ 40 K, whereas it becomes positive for low temperatures ≤ ~ 40 K, which implies an interplay of quantum interferences in Dirac materials. The elastic scattering mechanism in hBN/Gr/hBN stacks contrasts with that of conventional graphene on SiO2, and our ultra-clean graphene device shows nonzero magnetoconductance for high temperatures of up to 300 K.

In situ electron microscopy is an effective tool for understanding the mechanisms driving novel phenomena in 2D structures. However, due to practical challenges, it is difficult to address these technologically relevant 2D heterostructures with electron microscopy. Here, we use the differential phase contrast (DPC) imaging technique to build a methodology for probing local electrostatic fields during electrical operation with nanoscale spatial resolution in such materials. We find that, by combining a traditional DPC setup with a high-pass filter, we can largely eliminate electric fluctuations emanating from short-range atomic potentials. Using a method based on this filtering algorithm, a priori electric field expectations can be directly compared with experimentally derived values to readily identify inhomogeneities and potentially problematic regions. We use this platform to analyze the electric field and charge density distribution across layers of hBN and MoS(2).

Conducting materials typically exhibit either diffusive or ballistic charge transport. When electron–electron interactions dominate, a hydrodynamic regime with viscous charge flow emerges1–13. More stringent conditions eventually yield a quantum-critical Dirac-fluid regime, where electronic heat can flow more efficiently than charge14–22. However, observing and controlling the flow of electronic heat in the hydrodynamic regime at room temperature has so far remained elusive. Here we observe heat transport in graphene in the diffusive and hydrodynamic regimes, and report a controllable transition to the Dirac-fluid regime at room temperature, using carrier temperature and carrier density as control knobs. We introduce the technique of spatiotemporal thermoelectric microscopy with femtosecond temporal and nanometre spatial resolution, which allows for tracking electronic heat spreading. In the diffusive regime, we find a thermal diffusivity of roughly 2,000 cm2 s−1, consistent with charge transport. Moreover, within the hydrodynamic time window before momentum relaxation, we observe heat spreading corresponding to a giant diffusivity up to 70,000 cm2 s−1, indicative of a Dirac fluid. Our results offer the possibility of further exploration of these interesting physical phenomena and their potential applications in nanoscale thermal management., Spatiotemporal thermoelectric microscopy enables the observation of electronic heat flow in graphene in diffusive and hydrodynamic regimes at room temperature, as well as a controlled transition from a Fermi liquid to Dirac fluid.

Funding Information: We are grateful to B. J. Irving for carefully reading the manuscript. G.Z. thanks the National Science Foundation of China (NSFC, grant nos 11834017 and 61888102) and the Strategic Priority Research Program of CAS (grant no. XDB30000000) for their support. M.L. thanks the ESI Fund and the OPR DE International Mobility of Researchers MSCA-IF III at CTU in Prague (no. CZ.02.2.69/0.0/0.0/20_079/0017983) for their support. L.D. gratefully acknowledges the financial support from the Academy of Finland (grant no. 3333099). D.S. thanks the support from NSFC (grant no. 61734001). K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, A3 Foresight by JSPS and the CREST (JPMJCR15F3), JST. M.L., P.N. and T.P. acknowledge support from the project Novel Nanostructures for Engineering Applications CZ.02.1.01/0.0/0.0/16_026/0008396. This work was supported by the Ministry of Education, Youth and Sports of the Czech Republic through the e-INFRA CZ (ID:90140). T.P., V.E.P.C. and A.S. acknowledge support from the European Union’s Horizon 2020 research and innovation program under grant agreement no. 721642: SOLUTION. The data and materials are available from the corresponding authors upon request. The authors acknowledge the use of the IRIDIS High Performance Computing Facility, and associated support services at the University of Southampton, in the completion of this work. Publisher Copyright: © 2021, The Author(s), under exclusive licence to Springer Nature Limited. MoS2/graphite and MoS2/h-BN interfaces are shown to have ultra-low friction coefficients, whereas edges and interface steps mainly contribute to the friction force. Two-dimensional heterostructures are excellent platforms to realize twist-angle-independent ultra-low friction due to their weak interlayer van der Waals interactions and natural lattice mismatch. However, for finite-size interfaces, the effect of domain edges on the friction process remains unclear. Here we report the superlubricity phenomenon and the edge-pinning effect at MoS2/graphite and MoS2/hexagonal boron nitride van der Waals heterostructure interfaces. We found that the friction coefficients of these heterostructures are below 10(-6). Molecular dynamics simulations corroborate the experiments, which highlights the contribution of edges and interface steps to friction forces. Our experiments and simulations provide more information on the sliding mechanism of finite low-dimensional structures, which is vital to understand the friction process of laminar solid lubricants.

MoSe2–WSe2 heterostructures host strongly bound interlayer excitons (IXs), which exhibit bright photoluminescence (PL) when the twist angle is near 0° or 60°. Over the past several years, there have been numerous reports on the optical response of these heterostructures but no unifying model to understand the dynamics of IXs and their temperature dependence. Here we perform a comprehensive study of the temperature, excitation power, and time-dependent PL of IXs. We observe a significant decrease in PL intensity above a transition temperature that we attribute to a transition from localized to delocalized IXs. Astoundingly, we find a simple inverse relationship between the IX PL energy and the transition temperature, which exhibits opposite power-dependent behaviors for near 0° and 60° samples. We conclude that this temperature dependence is a result of IX–IX exchange interactions, whose effect is suppressed by the moiré potential trapping IXs at low temperature.

Chemical vapor deposition (CVD)-grown flakes of high-quality monolayers of WS2 can be stabilized at elevated temperatures by encapsulation with several layer hexagonal boron nitride (h-BN), but to different degrees in the presence of ambient air, flowing N2, and flowing forming gas (95% N2, 5% H2). The best passivation of WS2 at elevated temperature occurs for h-BN-covered samples with flowing N2 (after heating to 873 K), as judged by optical microscopy and photoluminescence (PL) intensity after a heating/cooling cycle. Stability is worse for uncovered samples, but best with flowing forming gas. PL from trions, in addition to that from excitons, is seen for covered WS2 only for forming gas, during cooling below ∼323 K; the trion has an estimated binding energy of ∼28 meV. It might occur because of doping level changes caused by charge defect generation by H2 molecules diffusing between the h-BN and the SiO2/Si substrate. The decomposition of uncovered WS2 flakes in air suggests a dissociation and chemisorption energy barrier of O2 on the WS2 surface of ∼1.6 eV. Fitting the high-temperature PL intensities in air gives a binding energy of a free exciton of ∼229 meV.

Recent advances in the manipulation and control of layered, two-dimensional materials has given way to the construction of heterostructures with new functionality and unprecedented electronic properties. In this study, we present a simple technique to assemble and transfer van der Waals heterostructures using common nail polish. Commercially available nail polish acts as a resilient sticky polymer, allowing for the fabrication of complex multi-material stacks without noticeable fatigue. Directly comparing four commercially available brands of nail polish, we find that one stands out in terms of stability and stacking characteristics. Using this method, we fabricate two top-gated devices and report their electrical properties. Our technique reduces the complexity in assembling van der Waals heterostructures based on the proven van der Waals pick up method.

Impurity doping is a viable route toward achieving desired subgap optical response in semiconductors. In strongly excitonic two-dimensional (2D) semiconductors such as transition metal dichalcogenides (TMDs), impurities are expected to result in bound-exciton emission. However, doped TMDs often exhibit a broad Stokes-shifted emission without characteristic features, hampering strategic materials engineering. Here we report observation of a well-defined impurity-induced emission in monolayer WS2 substitutionally doped with rhenium (Re), which is an electron donor. The emission exhibits characteristics of localized states and dominates the spectrum up to 200 K. Gate dependence reveals that neutral impurity centers are responsible for the observed emission. Using GW-Bethe-Salpeter equation (GW-BSE) calculations, we attribute the emission to transitions between spin-split upper Re band and valence band edge.

The allotropic affinity for bulk silicon and unique electronic and optical properties make silicene a promising candidate for future high-performance devices compatible with mature complementary metal-oxide-semiconductor technology. However, silicene's outstanding properties are not preserved on its most prominent growth templates, due to strong substrate interactions and hybridization effects. In this letter, we report the optical properties of silicene epitaxially grown on Au(111). A novel in situ passivation methodology with few-layer hexagonal boron nitride enables detailed ex situ characterization at ambient conditions via μ-Raman spectroscopy and reflectance measurements. The optical properties of silicene on Au(111) appeared to be in accordance with the characteristics predicted theoretically for freestanding silicene, allowing the conclusion that its prominent electronic properties are preserved. The absorption features are, however, modified by many-body effects induced by the Au substrate due to an increased screening of electron-hole interactions.

Interlayer (IL) excitons, comprising electrons and holes residing in different layers of van der Waals bonded two-dimensional semiconductors, have opened new opportunities for room-temperature excitonic devices. So far, two-dimensional IL excitons have been realized in heterobilayers with type-II band alignment. However, the small oscillator strength of the resulting IL excitons and difficulties with producing heterostructures with definite crystal orientation over large areas have challenged the practical applicability of this design. Here, following the theoretical prediction and recent experimental confirmation of the existence of IL excitons in bilayer MoS2, we demonstrate the electrical control of such excitons up to room temperature. We find that the IL excitonic states preserve their large oscillator strength as their energies are manipulated by the electric field. We attribute this effect to the mixing of the pure IL excitons with intralayer excitons localized in a single layer. By applying an electric field perpendicular to the bilayer MoS2 crystal plane, excitons with IL character split into two peaks with an X-shaped field dependence as a clear fingerprint of the shift of the monolayer bands with respect to each other. Finally, we demonstrate the full control of the energies of IL excitons distributed homogeneously over a large area of our device. The existence of interlayer excitons with strong oscillator strength in bilayer MoS2 enables their electrical manipulation up to room temperature.

Heterobilayers of transition metal dichalcogenides (TMDCs) can form a moiré superlattice with flat minibands, which enables strong electron interaction and leads to various fascinating correlated states. These heterobilayers also host interlayer excitons in a type-II band alignment, in which optically excited electrons and holes reside on different layers but remain bound by the Coulomb interaction. Here we explore the unique setting of interlayer excitons interacting with strongly correlated electrons, and we show that the photoluminescence (PL) of interlayer excitons sensitively signals the onset of various correlated insulating states as the band filling is varied. When the system is in one of such states, the PL of interlayer excitons is relatively amplified at increased optical excitation power due to reduced mobility, and the valley polarization of interlayer excitons is enhanced. The moiré superlattice of the TMDC heterobilayer presents an exciting platform to engineer interlayer excitons through the periodic correlated electron states., Heterobilayers of transition metal dichalcogenides host moiré superlattices that give rise to strong electron interactions. Here, the authors study the photoluminescence from interlayer excitons in a WS2/WSe2 heterobilayer to reveal the onset of various correlated insulating states.

Many of graphene’s remarkable properties arise from its linear dispersion of the electronic states, forming a Dirac cone at the K points of the Brillouin zone. Silicene, the 2D allotrope of silicon, is also predicted to show a similar electronic band structure, with the addition of a tunable bandgap, induced by spin–orbit coupling. Because of these outstanding electronic properties, silicene is considered as a promising building block for next-generation electronic devices. Recently, it has been shown that silicene grown on Au(111) still possesses a Dirac cone, despite the interaction with the substrate. Here, to fully characterize the structure of this 2D material, we investigate the vibrational spectrum of a monolayer silicene grown on Au(111) by polarized Raman spectroscopy. To enable a detailed ex situ investigation, we passivated the silicene on Au(111) by encapsulating it under few layers hBN or graphene flakes. The observed spectrum is characterized by vibrational modes that are strongly red-shifted with respect to the ones expected for freestanding silicene. By comparing low-energy electron diffraction (LEED) patterns and Raman results with first-principles calculations, we show that the vibrational modes indicate a highly (>7%) biaxially strained silicene phase., This work was funded by the Fonds zur Förderung der Wissenschaftlichen Forschung (FWF), Austria (Project P29244-N27). We also acknowledge financial support by the Ministerio de Economía, Industria y Competitividad (MINECO) under Grant FEDER-MAT2017-90024-P and the Severo Ochoa Centres of Excellence Program under Grant CEX2019-000917-S, and by the Generalitat de Catalunya under Grant 2017 SGR 1506. The project i-LINK action LINKA20047 funded by CSIC is also acknowledged for financial support. R.R. acknowledges useful discussions with Mariusz Krawiec. CzechNanoLab Project LM2018110 funded by MEYS CR is gratefully acknowledged for the financial support of the measurements at CEITEC Nano Research Infrastructure. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, Grant JPMXP0112101001, JSPS KAKENHI Grant JP20H00354, and the CREST(JPMJCR15F3), JST.

On-chip spectrometers with compact footprints are being extensively investigated owing to their promising future in critical applications such as sensing, surveillance and spectral imaging. Most existing miniaturized spectrometers use large arrays of photodetection elements to capture different spectral components of incident light, from which its spectrum is reconstructed. Here, we demonstrate a mid-infrared spectrometer in the 2–9 µm spectral range, utilizing a single tunable black phosphorus photodetector with an active area footprint of only 9 × 16 µm2, along with a unique spectral learning procedure. Such a single-detector spectrometer has a compact size at the scale of the operational wavelength. Leveraging the wavelength and bias-dependent responsivity matrix learned from the spectra of a tunable blackbody source, we reconstruct unknown spectra from their corresponding photoresponse vectors. Enabled by the strong Stark effect and the tunable light–matter interactions in black phosphorus, our single-detector spectrometer shows remarkable potential in the reconstruction of the spectra of both monochromatic and broadband light. Furthermore, its ultracompact structure that is free from bulky interferometers and gratings, together with its electrically reconfigurable nature, may open up pathways towards on-chip mid-infrared spectroscopy and spectral imaging. A single-photodetector spectrometer based on black phosphorus is demonstrated in the wavelength range from 2 to 9 μm. The footprint is 9 × 16 μm2. The spectrometer is free from bulky interferometers and gratings, and is electrically reconfigurable.

Few-layer transition metal dichalcogenides (TMDs) exhibit out-of-plane wave function confinement with subband quantization. This phenomenon is totally absent in monolayer crystals and is regarded a...

Engineering interface polarization Many properties can emerge at the interface of van der Waals materials created by rotating the layers of a single material or by creating heterointerfaces between different materials. Akamatsu et al. formed an interface that intentionally broke in-plane inversion symmetry by combining crystals of tungsten diselenide with threefold rotational symmetry and black phosphorus with twofold rotational symmetry. This interface creates in-plane electronic polarization that results in a spontaneous photovoltaic effect only along the polarization direction. This effect was explained in terms of a shift current mechanism. Science , this issue p. 68

Van der Waals (vdW) heterostructures, consisting of a variety of low-dimensional materials, have great potential use in the design of a wide range of functional devices thanks to their atomically thin body and strong electrostatic tunability. Here, we demonstrate multi-functional indium selenide (InSe)/black phosphorous (BP) heterostructures encapsulated by hexagonal boron nitride. At a positive drain bias (VD), applied on the BP while the InSe is grounded, our heterostructures show an intermediate gate voltage (VBG) regime where the current hardly changes, working as a ternary transistor. By contrast, at a negative VD, the device shows strong negative differential transconductance characteristics; the peak current increases up to ~5 μA and the peak-to-valley current ratio reaches 1600 at VD = −2 V. Four-terminal measurements were performed on each layer, allowing us to separate the contributions of contact resistances and channel resistance. Moreover, multiple devices with different device structures and contacts were investigated, providing insight into the operation principle and performance optimization. We systematically investigated the influence of contact resistances, heterojunction resistance, channel resistance, and the thickness of BP on the detailed operational characteristics at different VD and VBG regimes.

Two-dimensional heterostructures have been extensively investigated as next-generation nonvolatile memory (NVM) devices. In the past decade, drastic performance improvements and further advanced functionalities have been demonstrated. However, this progress is not sufficiently supported by the understanding of their operations, obscuring the material and device structure design policy. Here, detailed operation mechanisms are elucidated by exploiting the floating gate (FG) voltage measurements. Systematic comparisons of MoTe2, WSe2, and MoS2 channel devices revealed that the tunneling behavior between the channel and FG is controlled by three kinds of current-limiting paths, i.e., tunneling barrier, 2D/metal contact, and p-n junction in the channel. Furthermore, the control experiment indicated that the access region in the device structure is required to achieve 2D channel/FG tunneling by preventing electrode/FG tunneling. The present understanding suggests that the ambipolar 2D-based FG-type NVM device with the access region is suitable for further realizing potentially high electrical reliability.

In moir\'e crystals formed by stacking van der Waals (vdW) materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS$_2$ twisted bilayers, adding a new perspective to moir\'e physics. Over a range of small twist angles, the phonon spectra evolve rapidly due to ultra-strong coupling between different phonon modes and atomic reconstructions of the moir\'e pattern. We develop a new low-energy continuum model for phonons that overcomes the outstanding challenge of calculating properties of large moir\'e supercells and successfully captures essential experimental observations. Remarkably, simple optical spectroscopy experiments can provide information on strain and lattice distortions in moir\'e crystals with nanometer-size supercells. The newly developed theory promotes a comprehensive and unified understanding of structural, optical, and electronic properties of moir\'e superlattices., Comment: 21 pages, 4 figures

Graphene nanoribbons are predicted to support low-loss and tunable plasmonic waveguide modes with an ultrasmall mode area. Experimental observation of the plasmonic waveguide modes in graphene nanoribbons, however, is challenging because conventional wet lithography has difficulty creating a clean graphene nanoribbon with a low edge roughness. Here, we use a dry lithography method to fabricate ultraclean and low-roughness graphene nanoribbons, which are then encapsulated in hexagonal boron nitride (hBN). We demonstrate low-loss plasmon propagation with a quality factor up to 35 in the ultraclean nanoribbon waveguide using cryogenic infrared nanoscopy. In addition, we observe both the fundamental and the higher-order plasmonic waveguide modes for the first time. All the plasmon waveguide modes can be tuned through electrostatic gating. The observed tunable plasmon waveguide modes in ultraclean graphene nanoribbons agree well with the finite-difference time-domain (FDTD) simulation results. They are promising for reconfigurable photonic circuits and devices at a subwavelength scale.

Crystalline two-dimensional (2D) superconductors (SCs) with low carrier density are an exciting new class of materials in which electrostatic gating can tune superconductivity, electronic interactions play a prominent role, and electrical transport properties may directly reflect the topology of the Fermi surface. Here, we report the dramatic enhancement of superconductivity with decreasing thickness in semimetallic Td-MoTe2, with critical temperature (Tc) increasing up to 7.6 K for monolayers, a 60-fold increase with respect to the bulk Tc. We show that monolayers possess a similar electronic structure and density of states (DOS) as the bulk, implying that electronic interactions play a strong role in the enhanced superconductivity. Reflecting the low carrier density, the critical temperature, magnetic field, and current density are all tunable by an applied gate voltage. The response to high in-plane magnetic fields is distinct from that of other 2D SCs and reflects the canted spin texture of the electron pockets.

We investigate the origin of emission lines apparent in the low-temperature photoluminescence spectra of $n$-doped WS$_2$ monolayer embedded in hexagonal BN layers using external magnetic fields and first-principles calculations. Apart from the neutral A exciton line, all observed emission lines are related to the negatively charged excitons. Consequently, we identify emissions due to both the bright (singlet and triplet) and dark (spin- and momentum-forbidden) negative trions as well as the phonon replicas of the latter optically-inactive complexes. The semi-dark trions and negative biexcitons are distinguished. Based on their experimentally extracted and theoretically calculated $g$-factors, we identify three distinct families of emissions due to exciton complexes in WS$_2$: bright, intravalley and intervalley dark. The $g$-factors of the spin-split subbands in both the conduction and valence bands are also determined., Manuscript: 7 pages, 5 figures; SI: 5 pages, 3 figures

Complementary metal–oxide–semiconductor (CMOS) logic circuits at their ultimate scaling limits place extreme demands on the properties of all materials involved. The requirements for semiconductors are well explored and could possibly be satisfied by a number of layered two-dimensional (2D) materials, such as transition metal dichalcogenides or black phosphorus. The requirements for gate insulators are arguably even more challenging. At present, hexagonal boron nitride (hBN) is the most common 2D insulator and is widely considered to be the most promising gate insulator in 2D material-based transistors. Here we assess the material parameters and performance limits of hBN. We compare experimental and theoretical tunnel currents through ultrathin layers (equivalent oxide thickness of less than 1 nm) of hBN and other 2D gate insulators, including the ideal case of defect-free hBN. Though its properties make hBN a candidate for many applications in 2D nanoelectronics, excessive leakage currents lead us to conclude that hBN is unlikely to be suitable for use as a gate insulator in ultrascaled CMOS devices. This Perspective assesses the performance limits of hexagonal boron nitride when used as a gate insulator in complementary metal–oxide–semiconductor (CMOS) devices based on two-dimensional materials, concluding that due to excessive leakage currents, the material is unlikely to be suitable for use in ultrascaled CMOS devices.

Control of materials properties has been the driving force of modern technologies. So far, materials properties have been modulated by their composition, structure, and size. Here, by using cathodoluminescence in a scanning transmission electron microscope, we show that the optical properties of stacked,100 nm thick hexagonal boron nitride (hBN) films can be continuously tuned by their relative twist angles. Due to the formation of a moiré superlattice between the two interface layers of the twisted films, a new moiré sub-band gap is formed with continuously decreasing magnitude as a function of the twist angle, resulting in tunable luminescence wavelength and intensity increase of40×. Our results demonstrate that moiré phenomena extend beyond monolayer-based systems and can be preserved in a technologically relevant, bulklike material at room temperature, dominating optical properties of hBN films for applications in medicine, environmental, or information technologies.

Twisted bilayer heterostructures (TBHs) are materials whose physical properties depend on the twist angle between the two layers of two-dimensional (2D) materials. Those heterostructures are not fo...

Patterning graphene with a spatially periodic potential provides a powerful means to modify its electronic properties1–3. In particular, in twisted bilayers, coupling to the resulting moire superlattice yields an isolated flat band that hosts correlated many-body phases4,5. However, both the symmetry and strength of the effective moire potential are constrained by the constituent crystals, limiting its tunability. Here, we have exploited the technique of dielectric patterning6 to subject graphene to a one-dimensional electrostatic superlattice (SL)1. We observed the emergence of multiple Dirac cones and found evidence that with increasing SL potential the main and satellite Dirac cones are sequentially flattened in the direction parallel to the SL basis vector, behaviour resulting from the interaction between the one-dimensional SL electric potential and the massless Dirac fermions hosted by graphene. Our results demonstrate the ability to induce tunable anisotropy in high-mobility two-dimensional materials, a long-desired property for novel electronic and optical applications7,8. Moreover, these findings offer a new approach to engineering flat energy bands where electron interactions can lead to emergent properties9. Dielectric patterning allows tunable anisotropy in high-mobility one-dimensional graphene electrostatic superlattices.

Moire superlattices in transition metal dichalcogenide (TMD) heterostructures can host novel correlated quantum phenomena due to the interplay of narrow moire flat bands and strong, long-range Coulomb interactions1–9. However, microscopic knowledge of the atomically reconstructed moire superlattice and resulting flat bands is still lacking, which is critical for fundamental understanding and control of the correlated moire phenomena. Here we quantitatively study the moire flat bands in three-dimensional (3D) reconstructed WSe2/WS2 moire superlattices by comparing scanning tunnelling spectroscopy (STS) of high-quality exfoliated TMD heterostructure devices with ab initio simulations of TMD moire superlattices. A strong 3D buckling reconstruction accompanied by large in-plane strain redistribution is identified in our WSe2/WS2 moire heterostructures. STS imaging demonstrates that this results in a remarkably narrow and highly localized K-point moire flat band at the valence band edge of the heterostructure. A series of moire flat bands are observed at different energies that exhibit varying degrees of localization. Our observations contradict previous simplified theoretical models but agree quantitatively with ab initio simulations that fully capture the 3D structural reconstruction. Our results reveal that the strain redistribution and 3D buckling in TMD heterostructures dominate the effective moire potential and the corresponding moire flat bands at the Brillouin zone K points. Scanning tunnelling spectroscopy and ab initio simulations reveal buckling reconstruction and in-plane strain redistribution in WSe2/WS2 moire heterostructures.

We report, for the first time, that the oxidation of bilayer graphene (BLG) can be reversibly and stacking-specifically controlled. The infrared (IR) absorption, IR nanoscopy, and Raman spectroscop...

Two-dimensional transition metal dichalcogenide semiconductors are very promising candidates for future electronic applications with low power consumption due to a low leakage current and high on-off current ratio. In this study, we suggest a complementary circuit consisting of ambipolar WSe2 and n-MoS2 field-effect transistors (FETs), which demonstrate dual functions of a frequency doubler and single inversion AND (SAND) logic gate. In order to reduce the power consumption, a high-quality thin h-BN single crystal is used as a gate dielectric that leads to a low operating voltage of less than 5 V. By combining the low operating voltage with a low operating current in the complementary circuit, a low power consumption of 300 nW (a minimum of 10 pW) has been achieved, which is a significant improvement compared to the tens of μW consumed by a graphene channel. The complementary circuit shows the effective frequency doubling of the input with a dynamic range from 20 to 100 Hz. Furthermore, this circuit satisfies all the truth tables of a SAND logic gate that can be used as a universal logic gate like NAND. Considering that the NAND logic gate generally consists of four transistors, it is significantly advantageous to implement the equivalent circuit SAND logic gate with only two FETs. Our results open up possibilities for analog- and logic-circuit applications based on low-dimensional semiconductors.

Two-dimensional (2D) materials and heterostructures are promising candidates for nanoelectronics. However, the quality of material interfaces often limits the performance of electronic devices made from atomically thick 2D materials and heterostructures. Atomic force microscopy (AFM) tip-based cleaning is a reliable technique to remove interface contaminants and flatten heterostructures. Here, we demonstrate AFM tip-based cleaning applied to hBN-encapsulated monolayer MoS2 transistors, which results in electrical performance improvements of the devices. To investigate the impact of cleaning on device performance, we compared the characteristics of as-transferred heterostructures and transistors before and after tip-based cleaning using photoluminescence (PL) and electronic measurements. The PL linewidth of monolayer MoS2 decreased from 84 meV before cleaning to 71 meV after cleaning. The extrinsic mobility of monolayer MoS2 field-effect transistors increased from 21 cm2/Vs before cleaning to 38 cm2/Vs after cleaning. Using the results from AFM topography, photoluminescence, and back-gated field-effect measurements, we infer that tip-based cleaning enhances the mobility of hBN-encapsulated monolayer MoS2 by reducing interface disorder. Finally, we fabricate a MoS2 field-effect transistor (FET) from a tip-cleaned heterostructure and achieved a device mobility of 73 cm2/Vs. The results of this work could be used to improve the electrical performance of heterostructure devices and other types of mechanically assembled van der Waals heterostructures.

Semiconductors have long been perceived as a prerequisite for solid-state transistors. Although switching principles for nanometer-scale devices have emerged based on the deployment of two-dimensional (2D) van der Waals heterostructures, tunneling and ballistic currents through short channels are difficult to control, and semiconducting channel materials remain indispensable for practical switching. In this study, we report a semiconductor-less solid-state electronic device that exhibits an industry-applicable switching of the ballistic current. This device modulates the field emission barrier height across the graphene-hexagonal boron nitride interface with ION/IOFF of 106 obtained from the transfer curves and adjustable intrinsic gain up to 4, and exhibits unprecedented current stability in temperature range of 15–400 K. The vertical device operation can be optimized with the capacitive coupling in the device geometry. The semiconductor-less switching resolves the long-standing issue of temperature-dependent device performance, thereby extending the potential of 2D van der Waals devices to applications in extreme environments. In field-effect transistors, a semiconducting channel is indispensable for device switching. Here, the authors demonstrate semiconductor-less switching via modulation of the field emission barrier height across a graphene-hBN interface with ON/OFF ratio of 106.