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 between heterostructure and substrate. Crucially, we have found that interfacial thermal conductance between hBN and encapsulated MoS2 is 74MW/m2K and 72MW/m2K in supported and suspended films, respectively, which are significantly higher than interfacial thermal conductance between MoS2 and other substrates. Molecular dynamics (MD) computations conducted in parallel have shown consistent results. This work provides clear evidence of significantly efficient heat dissipation in hBN/MoS2/hBN heterostructures and sheds light on building novel hBN encapsulated nanoelectronics with efficient thermal management.
Graphene sheets encapsulated between hexagonal Boron Nitride (hBN) slabs display superb electronic properties due to very limited scattering from extrinsic disorder sources such as Coulomb impurities and corrugations. Such samples are therefore expected to be ideal platforms for highly-tunable low-loss plasmonics in a wide spectral range. In this Article we present a theory of collective electron density oscillations in a graphene sheet encapsulated between two hBN semi-infinite slabs (hBN/G/hBN). Graphene plasmons hybridize with hBN optical phonons forming hybrid plasmon-phonon (HPP) modes. W…
We present measurements of temperature dependence of photoluminescence intensity from monolayer MoS2 encapsulated by hexagonal boron nitride (hBN) flakes. The obtained temperature dependence shows an opposite trend to that of previously observed in a monolayer MoS2 on a SiO2 substrate. Ab-initio bandstructure calculations have revealed that monolayer MoS2 encapsulated by hBN flakes have no longer a direct-gap semiconductor but an indirect-gap semiconductor. This is caused by orbital hybridization between MoS2 and hBN, which leads to upward shift of gamma-valley of MoS2. This work shows an impo…
Excitons, quasi particles composed of an electron and a hole, play an important role in optical responses in low-dimensional nanostructures. In this work, we have investigated exciton diffusion in a monolayer MoSe2 encapsulated between flakes of hexagonal boron nitrides (hBN/MoSe2/hBN). Through PL imaging and numerical solving the 2D diffusion equation, we revealed that temperature dependence of exciton mobility in the hBN/MoSe2/hBN shows non-saturating increase at low temperature, which is qualitatively different from those of quantum wells composed of compound semiconductors. Ultraflat struc…
We study fully hexagonal boron nitride (hBN)-encapsulated graphene spin valve devices at room temperature. The device consists of a graphene channel encapsulated between two crystalline hBN flakes; thick-hBN flake as a bottom gate dielectric substrate which masks the charge impurities from SiO2/Si substrate and single-layer thin-hBN flake as a tunnel barrier. Full encapsulation prevents the graphene from coming in contact with any polymer/chemical during the lithography and thus gives homogeneous charge and spin transport properties across different regions of the encapsulated graphene. Furthe…
Atomically thin materials, like semiconducting transition metal dichalcogenides, are highly sensitive to the environment. This opens up an opportunity to externally control their properties by changing their surroundings. In this work, high-quality van der Waals heterostructures assembled from hBN-encapsulated monolayer MoS$_2$ are studied with the aid of photoluminescence, photoluminescence excitation, and reflectance contrast experiments. We demonstrate that carrier concentration in MoS$_2$ monolayers, arising from charge transfer from impurities in the substrate, can be significantly tuned …
Low frequency 1/f noise is investigated in graphene, encapsulated between hexagonal boron nitride (hBN) substrate in dual gated geometry. The overall noise magnitude is smaller as compared to graphene on Si/SiO2 substrate. The noise amplitude in the hole doped region is independent of carrier density while in the electron doped region, a pronounced peak is observed, at Fermi energy, EF ~ 90 meV. The physical mechanism of the anomalous noise peak in the electron doped region is attributed to the impurity states originating from the Carbon atom replacing the Nitrogen site in hBN crystal. Further…
New techniques for probing hyperbolic phonon polaritons (HPP) in 2D materials will support the development of the emerging technologies in this field. Previous reports have shown that it is possible for WSe2 monolayers in contact with the hexagonal boron nitride (hBN) to generate HPP in the hBN via Raman scattering. In this paper, we set out new results on HPP Raman scattering induced in hBN by WSe2 and MoSe2 monolayers including new resonances at which the Raman scattering is enhanced. Analysis of the observed Raman lineshapes demonstrates that Raman scattering allows HPP with wavevectors wit…
The excellent electronic and mechanical properties of graphene allow it to sustain very large currents, enabling its incandescence through Joule heating in suspended devices. Although interesting scientifically and promising technologically, this process is unattainable in ambient environment, because graphene quickly oxidises at high temperatures. Here, we take the performance of graphene-based incandescent devices to the next level by encapsulating graphene with hexagonal boron nitride (hBN). Remarkably, we found that the hBN encapsulation provides an excellent protection for hot graphene fi…
Researchers are currently exploring nanoporous two-dimensional materials, such as hexagonal boron nitride (hBN), as potential desalination membranes. Here, we study the effect of grain boundaries (GBs) and interfacial electrostatic interactions on the desalination performance of bicrystalline nanoporous hBN, using classical molecular dynamics simulations supported by quantum-mechanical density functional theory (DFT) calculations. We investigate three different nanoporous bicrystalline hBN configurations, with symmetric tilt GBs having misorientation angles of 13.2°, 21.8°, and 32.2°. We find …
We use confocal Raman microscopy and modified vector analysis methods to investigate the nanoscale origin of strain and carrier concentration in exfoliated graphene-hexagonal boron nitride (hBN) heterostructures on silicon dioxide (SiO2). Two types of heterostructures are studied: graphene on SiO2 partially coved by hBN, and graphene fully encapsulated between two hBN flakes. We extend the vector analysis methods to produce spatial maps of the strain and doping variation across the heterostructures. This allows us to visualise and directly quantify the much-speculated effect of the environment…
Using a simple setup to bend a flexible substrate, we demonstrate deterministic and reproducible in-situ strain tuning of graphene electronic devices. Central to this method is the full hBN encapsulation of graphene, which preserves the exceptional quality of pristine graphene for transport experiments. In addition, the on-substrate approach allows one to exploit strain effects in the full range of possible sample geometries and at the same time guarantees that changes in the gate capacitance remain negligible during the deformation process. We use Raman spectroscopy to spatially map the strai…
We investigate the zero-bias behavior of Josephson junctions made of encapsulated graphene boron nitride heterostructures in the long ballistic junction regime. For temperatures down to 2.7K, the junctions appear non-hysteretic with respect to the switching and retrapping currents $I_C$ and $I_R$. A small non-zero resistance is observed even around zero bias current, and scales with temperature as dictated by the phase diffusion mechanism. By varying the graphene carrier concentration we are able to confirm that the observed phase diffusion mechanism follows the trend for an overdamped Josephs…
Uncooled Terahertz (THz) photodetectors (PDs) showing fast (ps) response and high sensitivity (noise equivalent power (NEP) < $nWHz^{-1/2}$) over a broad (0.5THz-10THz) frequency range are needed for applications in high-resolution spectroscopy (relative accuracy ~ $10^{-11}$), metrology, quantum information, security, imaging, optical communications. However, present THz receivers cannot provide the required balance between sensitivity, speed, operation temperature and frequency range. Here, we demonstrate an uncooled THz PD combining the low (~2000 $k_{B}μm^{-2}$) electronic specific heat of…
We present a novel method to establish inner point contacts on hexagonal boron nitride (hBN) encapsulated graphene heterostructures with dimensions as small as 100 nm by pre-patterning the top-hBN in a separate step prior to dry-stacking. 2 and 4-terminal field effect measurements between different lead combinations are in qualitative agreement with an electrostatic model assuming pointlike contacts. The measured contact resistances are 0.5-1.5 k$Ω$ per contact, which is quite low for such small contacts. By applying a perpendicular magnetic fields, an insulating behaviour in the quantum Hall …
Observation of Unconventional Ferroelectricity in Non-Moir'\e Graphene on Hexagonal Boron Nitride Boundaries and Interfaces
The University of Hong Kong（香港大学）；HK Institute of Quantum Science & Technology, The University of Hong Kong（香港大学量子科学与技术研究所）；National Institute for Materials Science（物质材料研究机构）
Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of nonlocal interactions of \textit{free} trions in pristine hBN/MoS$_2$/hBN heterostructures coupled to single mode (Q $>10^4$) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stems from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS$_2$ monolayer. We observ…
We study room temperature spin transport in graphene devices encapsulated between a layer-by-layer-stacked two-layer-thick chemical vapour deposition (CVD) grown hexagonal boron nitride (hBN) tunnel barrier, and a few-layer-thick exfoliated-hBN substrate. We find mobilities and spin-relaxation times comparable to that of SiO$_2$ substrate based graphene devices, and obtain a similar order of magnitude of spin relaxation rates for both the Elliott-Yafet and D'Yakonov-Perel' mechanisms. The behaviour of ferromagnet/two-layer-CVD-hBN/graphene/hBN contacts ranges from transparent to tunneling due …
Using time-resolved optical Kerr rotation, we measure the low temperature valley dynamics of resident electrons and holes in exfoliated WSe$_2$ monolayers as a systematic function of carrier density. In an effort to reconcile the many disparate timescales of carrier valley dynamics in monolayer semiconductors reported to date, we directly compare the doping-dependent valley relaxation in two electrostatically-gated WSe$_2$ monolayers having different dielectric environments. In a fully-encapsulated structure (hBN/WSe$_2$/hBN, where hBN is hexagonal boron nitride), valley relaxation is found to…
Hexagonal boron nitride is the only substrate that has so far allowed graphene devices exhibiting micron-scale ballistic transport. Can other atomically flat crystals be used as substrates for making quality graphene heterostructures? Here we report on our search for alternative substrates. The devices fabricated by encapsulating graphene with molybdenum or tungsten disulphides and hBN are found to exhibit consistently high carrier mobilities of about 60,000 cm$^{2}$V$^{-1}$s$^{-1}$. In contrast, encapsulation with atomically flat layered oxides such as mica, bismuth strontium calcium copper o…
To explore the potential of field-effect transistors (FETs) based on monolayers of the two-dimensional semiconducting channel(SC) for spintronics, the two most important issues are to ensure the formation of variable low resistive tunnel ferromagnetic contacts(FC), and to preserve intrinsic properties of the SC during fabrication. Large Schottky barriers lead to the formation of high resistive contacts and methods adopted to control the barriers often alter the intrinsic properties of the SC. This work aims at addressing both issues in fully encapsulated monolayer WSe$_2$ FETs by using bi-laye…
We develop the device model for the proposed injection (electrically) driven thermal light emitters (IDLEs) based on the vertical Hexagonal Boron Nitride Layer/Graphene Layer/ Hexagonal Boron Nitride Layer (hBNL/GL/hBNL) heterostructures and analyze their dynamic response. The operation of the IDLEs is associated with the light emission of the hot two-dimensional electron-hole plasma (2DEHP) generated in the GL by both the lateral injection from the side contacts and the vertical injection through the hBNL (combined injection) heating the 2DEHP. The temporal variation of the injection current …
A periodic spatial modulation, as created by a moiré pattern, has been extensively studied with the view to engineer and tune the properties of graphene. Graphene encapsulated by hexagonal boron nitride (hBN) when slightly misaligned with the top and bottom hBN layers experiences two interfering moiré patterns, resulting in a so-called super-moiré (SM). This leads to a lattice and electronic spectrum reconstruction. A geometrical construction of the non-relaxed SM patterns allows us to indicate qualitatively the induced changes in the electronic properties and to locate the SM features in the …
The strong light-matter interaction in transition Metal dichalcogenides (TMDs) monolayers (MLs) is governed by robust excitons. Important progress has been made to control the dielectric environment surrounding the MLs, especially through hexagonal boron nitride (hBN) encapsulation, which drastically reduces the inhomogeneous contribution to the exciton linewidth. Most studies use exfoliated hBN from high quality flakes grown under high pressure. In this work, we show that hBN grown by molecular beam epitaxy (MBE) over a large surface area substrate has a similarly positive impact on the optic…
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 specific rotational alignment of two-dimensional lattices results in a moiré superlattice with a larger period than the original lattices and allows one to engineer the electronic band structure of such materials. So far, transport signatures of such superlattices have been reported for graphene/hBN and graphene/graphene systems. Here we report moiré superlattices in fully hBN encapsulated graphene with both the top and the bottom hBN aligned to the graphene. In the graphene, two different moiré superlattices form with the top and the bottom hBN, respectively. The overlay of the two superl…
Among two-dimensional atomic crystals, hexagonal boron nitride (hBN) is one of the most remarkable materials to fabricate heterostructures revealing unusual properties. We perform first-principles calculations to determine whether intercalated metal atoms and vacancies can mediate interfacial coupling and influence the structural and electronic properties of the graphene/hBN heterostructure. Metal impurity atoms (Li, K, Cr, Mn, Co, and Cu) as extrinsic defects between the graphene and hBN sheets produce $n$-doped graphene. We also consider intrinsic vacancy defects and find that a boron monova…
We study spin transport in a fully hBN encapsulated monolayer-graphene van der Waals (vdW) heterostructure, at room temperature. A top-layer of bilayer-hBN is used as a tunnel barrier for spin-injection and detection in graphene with ferromagnetic cobalt electrodes. We report surprisingly large and bias induced (differential) spin-injection (detection) polarizations up to 50% (135%) at a positive voltage bias of +0.6 V, as well as sign inverted polarizations up to -70% (-60%) at a reverse bias of -0.4 V. This demonstrates the potential of bilayer-hBN tunnel barriers for practical graphene spin…
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…
Twistronic heterostructures have recently emerged as a new class of quantum electronic materials with properties determined by the twist angle between the adjacent two-dimensional materials. Here we study moiré superlattice minibands in graphene (G) encapsulated in hexagonal boron nitride (hBN) with an almost perfect alignment with both the top and bottom hBN crystals. We show that, for such an orientation of the unit cells of the hBN layers that locally breaks inversion symmetry of the graphene lattice, the hBN/G/hBN structure features a Kagomé network of topologically protected chiral states…
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 report on the fabrication and characterization of high-quality chemical vapor-deposited (CVD) bilayer graphene (BLG). In particular, we demonstrate that CVD-grown BLG can mechanically be detached from the copper foil by an hexagonal boron nitride (hBN) crystal after oxidation of the copper-to-BLG interface. Confocal Raman spectroscopy reveals an AB-stacking order of the BLG crystals and a high structural quality. From transport measurements on fully encapsulated hBN/BLG/hBN Hall bar devices we extract charge carrier mobilities up to 180,000 cm$^2$/(Vs) at 2 K and up to 40,000 cm$^2$/(Vs) at…
When using hexagonal boron-nitride (hBN) as a substrate for graphene, the resulting moiré pattern creates secondary Dirac points. By encapsulating a multilayer graphene within aligned hBN sheets the controlled moiré stacking may offer even richer benefits. Using advanced tight-binding simulations on atomistically-relaxed heterostructures, here we show that the gap at the secondary Dirac point can be opened in selected moiré-stacking configurations, and is independent of any additional vertical gating of the heterostructure. On the other hand, gating can broadly tune the gap at the principal Di…
Aqueous proton transport at interfaces is ubiquitous and crucial for a number of fields, ranging from cellular transport and signaling, to catalysis and membrane science. However, due to their light mass, small size and high chemical reactivity, uncovering single proton surface transport at room temperature and in aqueous environment has so far remained out-of-reach of conventional atomic-scale surface science techniques, such as STM. Here, we use single-molecule localization microscopy techniques to resolve optically the transport of individual excess protons at the interface of hexagonal bor…
Hysteresis-Free High Mobility Graphene Encapsulated in Tungsten Disulfide
ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（光子科学研究所，巴塞罗那科学技术研究院）；Department of Molecular Sciences and Nanosystems, Ca’ Foscari University of Venice（威尼斯大学分子科学与纳米系统系）；School for Engineering of Matter, Transport and Energy, Arizona State University（亚利桑那州立大学物质、交通与能源工程学院）
Electronic transport in BN-encasulated graphene limited by remote phonon scattering
Laboratoire Charles Coulomb (L2C), UMR 5221 CNRS-Université de Montpellier（蒙彼利埃大学查尔斯·库隆实验室）；Aix Marseille Univ, CNRS, CINaM, AMUTech（艾克斯马赛大学）；University of Modena and Reggio Emilia（摩德纳和雷焦艾米利亚大学）；Sapienza Università di Roma（罗马第一大学）
We demonstrate the reduction of the inhomogeneous linewidth of the free excitons in atomically thin transition metal dichalcogenides (TMDCs) MoSe$_{2}$, WSe$_{2}$ and MoS$_{2}$ by encapsulation within few nanometer thick hBN. Encapsulation is shown to result in a significant reduction of the 10K excitonic linewidths down to $\sim3.5 \text{ meV}$ for n-MoSe$_{2}$, $\sim5.0 \text{ meV}$ for p-WSe$_{2}$ and $\sim4.8 \text{ meV}$ for n-MoS$_{2}$. Evidence is obtained that the hBN environment effectively lowers the Fermi level since the relative spectral weight shifts towards the neutral exciton em…
We perform extensive first-principles calculations for heterostructures composed of monolayer graphene and hexagonal boron nitride (hBN). Employing a symmetry-derived minimal tight-binding model, we extract orbital and spin-orbit coupling (SOC) parameters for graphene on hBN, as well as for hBN encapsulated graphene. Our calculations show that the parameters depend on the specific stacking configuration of graphene on hBN. We also perform an interlayer distance study for the different graphene/hBN stacks to find the corresponding lowest energy distances. For very large interlayer distances, on…
Displacement-Field-Induced Ionization of Defect States in High-Quality hBN
National University of Singapore（新加坡国立大学）；Institute for Functional Intelligent Materials, National University of Singapore（新加坡国立大学功能智能材料研究所）；University of Manchester（曼彻斯特大学）；National Graphene Institute, University of Manchester（曼彻斯特大学国家石墨烯研究所）；University of Southampton（南安普顿大学）；National Institute for Materials Science（日本物质材料研究机构）
Suppressing Plasmonic Heating in Aqueous Environments with Hexagonal Boron Nitride
Eindhoven University of Technology（埃因霍温理工大学）；Institute of Complex Molecular Systems, Eindhoven University of Technology（埃因霍温理工大学复杂分子系统研究所）；Institut Fresnel, CNRS, Aix Marseille Univ, Centrale Med（法国国家科学研究中心艾克斯马赛大学中央理工马arseille学院菲涅尔研究所）；Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST（加泰罗尼亚纳米科学与技术研究所）
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 …
The intercalation-induced phase transition of MoS2 from the semiconducting 2H to the semimetallic 1T' phase has been studied in detail for nearly a decade; however, the effects of a heterointerface between MoS2 and other two-dimensional (2D) crystals on the phase transition have largely been overlooked. Here, ab initio calculations show that intercalating Li at a MoS2-hexagonal boron nitride (hBN) interface stabilizes the 1T phase over the 2H phase of MoS2 by ~ 100 mJ m-2, suggesting that encapsulating MoS2 with hBN may lower the electrochemical energy needed for the intercalation-induced phas…
Atomically thin materials are exceedingly susceptible to their dielectric environment. For transition metal dichalcogenides, sample placement on a substrate or encapsulation in hexagonal boron nitride (hBN) are frequently used. In this paper we show that the dielectric response due to optical phonons of adjacent materials influences excitons in 2d crystals. We provide an analytic model for the coupling of 2d charge carriers to optical substrate phonons, which causes polaron effects similar to that of intrinsic 2d phonons. We apply the model to hBN-encapsulated WSe2, finding a significant reduc…
We report the fabrication of hexagonal-boron-nitride (hBN) encapsulated multi-terminal WSe$_2$ Hall bars with 2D/2D low-temperature Ohmic contacts as a platform for investigating the two-dimensional (2D) metal-insulator transition. We demonstrate that the WSe$_2$ devices exhibit Ohmic behavior down to 0.25 K and at low enough excitation voltages to avoid current-heating effects. Additionally, the high-quality hBN-encapsulated WSe$_2$ devices in ideal Hall-bar geometry enable us to accurately determine the carrier density. Measurements of the temperature ($T$) and density ($n_s$) dependence of …
Large spin-orbital proximity effects have been predicted in graphene interfaced with a transition metal dichalcogenide layer. Whereas clear evidence for an enhanced spin-orbit coupling has been found at large carrier densities, the type of spin-orbit coupling and its relaxation mechanism remained unknown. We show for the first time an increased spin-orbit coupling close to the charge neutrality point in graphene, where topological states are expected to appear. Single layer graphene encapsulated between the transition metal dichalcogenide WSe$_2$ and hBN is found to exhibit exceptional quality…
