Atomically thin semi-conductors are characterized by strongly bound excitons which govern the optical properties of the materials below and near the band edge. Efficient conversion of photons into electrical current requires, as a first step, the dissociation of the exciton into free electrons and holes. Here we calculate the dissociation rates of excitons in monolayer MoS$_2$ as a function of an applied in-plane electric field. The dissociation rates are obtained as the inverse lifetime of the resonant states of a two-dimensional Hydrogenic Hamiltonian which describes the exciton within the Mott-Wannier model. The resonances are computed using complex scaling, and the effective masses and screened electron-hole interaction defining the Hydrogenic Hamiltonian are computed from first-principles. For field strengths above 0.1 V/nm the dissociation lifetime is shorter than 1 picosecond, which is shorter than the lifetime of other, competing, decay mechanisms. Interestingly, encapsulation of the \moly layer in just two layers of hBN, enhances the dissociation rate by around one order of magnitude due to the increased screening showing that dielectric engineering is an effective way to control exciton lifetimes in two-dimensional materials.
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…
Monolayer transition metal dichalcogenides(2D) and zero dimensional quantum dots(QD) are known to have unique optical properties in their individual limit such as high binding energy of excitons. The combination of these two systems is of particular interest in understanding various aspects of energy transfer, charge transfer, dynamics of excitons, etc. In this manuscript, we report the anomalous photoluminescence(PL) emission in one such heterostructure MoS2-CdSe QD. We observe multiple exciton emission peaks of the heterostructure on hBN substrate which are absent on SiO2. Our observation op…
State-of-the-art fabrication and characterization techniques have been employed to measure the thermal conductivity of suspended, single-crystalline MoS2 and MoS2/hBN heterostructures. Two-laser Raman scattering thermometry was used combined with real time measurements of the absorbed laser power, which allowed us to determine the thermal conductivities without any assumptions. Measurements on MoS2 layers with thicknesses of 5 and 14 exhibit thermal conductivity in the range between 12 and 24 Wm-1K-1. Additionally, after determining the thermal conductivity of a selected MoS2 sample, an hBN fl…
Ultrafast charge transfer processes provide a facile way to create interlayer excitons in directly contacted transition metal dichalcogenide (TMD) layers. More sophisticated heterostructures composed of TMD/hBN/TMD enable new ways to control interlayer exciton properties and achieve novel exciton phenomena, such as exciton insulators and condensates, where longer lifetimes are desired. In this work, we experimentally study the charge transfer dynamics in a heterostructure composed of a 1 nm thick hBN spacer between MoSe$_{2}$ and WSe$_{2}$ monolayers. We observe the hole transfer from MoSe$_{2…
We report experimental and computational studies of thermal transport properties in hexagonal boron nitride (hBN) encapsulated molybdenum disulfide (MoS2) structure using refined optothermal Raman techniques, and reveal very high interfacial thermal conductance between hBN and MoS2. By studying the Raman shift of hBN and MoS2 in suspended and substrate-supported thin films under varying laser power and temperature, we calibrate lateral (in-plane) thermal conductivity of hBN and MoS2 and the vertical interfacial thermal conductance in the hBN/MoS2/hBN heterostructure as well as the interfaces b…
Atomically thin materials, like semiconducting transition metal dichalcogenides, are highly sensitive to the environment. This opens up an opportunity to externally control their properties by changing their surroundings. In this work, high-quality van der Waals heterostructures assembled from hBN-encapsulated monolayer MoS$_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 …
Recent works have revealed that van der Waals (vdW) epitaxial growth of 2D materials on crystalline substrates, such as hexagonal boron nitride (hBN), leads to formation of self-aligned grains, which results in defect-free stitching between the grains. However, how the weak vdW interaction causes strong limitation on orientation of grains is still not understood yet. In this work, we have focused on investigation of mechanism of self-alignment of MoS2 grains in vdW epitaxial growth on hBN. Through calculation based on density functional theory and the Lennard-Jones potential, we found that int…
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…
Complementary metal oxide semiconductor (CMOS) logic circuits at the ultimate scaling limit place the utmost 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, like for example transition-metal dichalcogenides or black phosphorus. The requirements for the gate insulator are arguably even more challenging and difficult to meet. In particular the combination of insulator to semiconductor which forms the central element of the metal oxide semiconductor fie…
Graphene on hBN (G/hBN) has a long period moiré superstructure owing to the lattice mismatch between two materials. Long periodic potential caused by the moiré superstructure induces modulation of electronic properties of the system. In this paper, we numerically calculate optical conductivity of G/hBN under circularly polarized light irradiation. The lack of spatial inversion symmetry in G/hBN induces the valley polarization. In further, the valley polarization becomes most pronounced in the infrared and terahertz regions if the twist angle between two materials is close to zero for non-dopin…
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…
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…
Two dimensional materials and their heterostructures constitute a promising platform to study correlated electronic states as well as many body physics of excitons. Here, we present experiments that unite these hitherto separate efforts and show how excitons that are dynamically screened by itinerant electrons to form exciton-polarons, can be used as a spectroscopic tool to study interaction-induced incompressible states of electrons. The MoSe$_2$/hBN/MoSe$_2$ heterostructure that we study exhibits a long-period Moiré superlattice as evidenced by coherent-hole tunneling mediated avoided crossi…
Calculating the quasiparticle (QP) band structure of two-dimensional (2D) materials within the GW self-energy approximation has proven to be a rather demanding computational task. The main reason is the strong $\mathbf{q}$-dependence of the 2D dielectric function around $\mathbf{q} = \mathbf{0}$ that calls for a much denser sampling of the Brillouin zone than is necessary for similar 3D solids. Here we use an analytical expression for the small $\mathbf{q}$-limit of the 2D response function to perform the BZ integral over the critical region around $\mathbf{q} = \mathbf{0}$. This drastically r…
In van der Waals heterostructures, the relative alignment of bands between layers, and the resulting band hybridisation, are key factors in determining a range of electronic properties. This work examines these effects for heterostructures of transition metal dichalcogenides (TMDs) and hexagonal boron nitride (hBN), an ubiquitous combination given the role of hBN as an encapsulating material. By comparing results of density functional calculations with experimental angle-resolved photoemission spectroscopy (ARPES) results, we explore the hybridisation between the valence states of the TMD and …
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…
Large, high-quality layers of hexagonal boron nitride (hBN) are a prerequisite for further advancement in scientific investigation and technological utilization of this exceptional 2D material. Here we address this demand by investigating chemical vapor deposition synthesis of hBN on an Ir(111) substrate, and focus on the substrate morphology, more specifically mono-atomic steps that are always present on all catalytic surfaces of practical use. From low-energy electron microscopy and atomic force microscopy data, we are able to set up an extended Wulff construction scheme and provide a clear …
Combined diverse two-dimensional (2D) materials for semiconductor interfaces are attractive for electrically controllable carrier confinement to enable excellent electrostatic control. We investigated the transport characteristic in heterointerface of multilayer molybdenum disulfide and hexagonal boron nitride (MoS$_2$/h-BN) to reveal that the charge transfer switching (CTS) is highly dependent on both the local gate constriction and bias in the channel. Notably, the CTS is shown to be controlled at a molecular level through electrotunable gated constriction. The resulting significant change i…
Light-matter interaction in two-dimension photonic materials allows for confinement and control of free-space radiation on sub-wavelength scales. Most notably, the van der Waals heterostructure obtained by stacking graphene (G) and hexagonal Boron Nitride (hBN) can provide for hybrid hyperbolic plasmon phonon-polaritons (HP3). Here, we present a polariton diode effect and low-bias control of HP3 modes confined in G-hBN. Using broadband infrared synchrotron radiation coupled to a scattering-type near-field optical microscope, we launch HP3 waves over both hBN Reststrahlen bands and observe the …
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…
Van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed dimensional p-n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS2 (2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. Here, we study the kinetics of excited carriers in pentacene-MoS2 p-n type-II heter…
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…
Graphene/hBN heterostructures can be considered as one of the basic building blocks for the next-generation optoelectronics mostly owing to the record-high electron mobilities. However, currently, the studies of the intrinsic optical properties of graphene are limited to the standard substrates (SiO2/Si, glass, quartz) despite the growing interest in graphene/hBN heterostructures. This can be attributed to a challenging task of the determination of hBN's strongly anisotropic dielectric tensor in the total optical response. In this study, we overcome this issue through imaging spectroscopic ell…
Photoexcited intralayer excitons in van der Waals heterostructures (vdWHs) with type-II band alignment have been observed to tunnel into interlayer excitons on ultrafast timescales. Such interlayer excitons have sufficiently long lifetimes that inducing dissociation with external in-plane electric fields becomes an attractive option of improving efficiency of photocurrent devices. In the present paper, we calculate interlayer exciton binding energies, Stark shifts, and dissociation rates for six different transition metal dichalcogenide (TMD) vdWHs using a numerical procedure based on exterior…
We investigate the proximity-induced exchange coupling in transition-metal dichalcogenides (TMDCs), originating from spin injector geometries composed of hexagonal boron-nitride (hBN) and ferromagnetic (FM) cobalt (Co) or nickel (Ni), from first-principles. We employ a minimal tight-binding Hamiltonian that captures the low energy bands of the TMDCs around K and K' valleys, to extract orbital, spin-orbit, and exchange parameters. The TMDC/hBN/FM heterostructure calculations show that due to the hBN buffer layer, the band structure of the TMDC is preserved, with an additional proximity-induced …
We undertook an ab-initio study of hexagonal boron nitride (hBN) sandwiched between Ni(111) layers to examine the interface of this material structure. We considered Ni(111)/hBN/Ni(111) with a slab with three Ni atomic layers to determine the exact atom arrangement at the interface. The density functional theory calculations for 36 stacking arrangements, which are doubled with respect to the magnetic alignment of slabs in an anti-parallel configuration (APC) and parallel configuration (PC), revealed that the number of formed weak chemical bonds, in the pd-hybridization between the N and Ni ato…
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…
Hexagonal boron nitride (hBN) is a wide bandgap van der Waals material that has recently emerged as promising platform for quantum photonics experiments. In this work we study the formation and localization of narrowband quantum emitters in large flakes (up to tens of microns wide) of hBN. The emitters can be activated in as-grown hBN by electron irradiation or high temperature annealing, and the emitter formation probability can be increased by ion implantation or focused laser irradiation of the as-grown material. Interestingly, we show that the emitters are always localized at edges of the …
We study anisotropies of helicity modulus, excitation spectrum, sound velocity and angle-resolved luminescence spectrum in a two-dimensional system of interacting excitons in a periodic potential. Analytical expressions for anisotropic corrections to the quantities characterizing superfluidity are obtained. We consider particularly the case of dipolar excitons in quantum wells. For GaAs/AlGaAs heterostructures as well as MoS$_2$/hBN/MoS$_2$ and MoSe$_2$/hBN/WSe$_2$ transition metal dichalcogenide bilayers estimates of the magnitude of the predicted effects are given. We also present a method t…
Layered materials can be assembled vertically to fabricate a new class of van der Waals (VDW) heterostructures a few atomic layers thick, compatible with a wide range of substrates and optoelectronic device geometries, enabling new strategies for control of light-matter coupling. Here, we incorporate molybdenum diselenide/boron nitride (MoSe$_2$/hBN) quantum wells (QWs) in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe$_2$ excitons and cavity photons, evidenced from a clear anticrossing between the neutra…
Generation of photocurrents in semiconducting materials requires dissociation of excitons into free charge carriers. While thermal agitation is sufficient to induce dissociation in most bulk materials, an additional push is required to induce efficient dissociation of the strongly bound excitons in monolayer transition-metal dichalcogenides (TMDs). Recently, static in-plane electric fields have proven to be a promising candidate. In the present paper, we introduce a numerical procedure, based on exterior complex scaling, capable of computing field-induced exciton dissociation rates for a wider…
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 b…
Strain in two-dimensional (2D) transition metal dichalcogenide (TMD) has led to localized states with exciting optical properties, in particular in view of designing one photon sources. The naturally formed of the MoS2 monolayer deposed on hBN substrate leads to a reduction of the bandgap in the strained region creating a nanobubble. The photogenerated particles are thus confined in the strain-induced potential. Using numerical diagonalization, we simulate the spectra of the confined exciton states, their oscillator strengths and radiative lifetimes. We show that a single state of the confined…
We demonstrate that, in monolayers (MLs) of semiconducting transition metal dichalcogenides, the $s$-type Rydberg series of excitonic states follows a simple energy ladder: $ε_n=-Ry^*/(n+δ)^2$, $n$=1,2,\ldots, in which $Ry^*$ is very close to the Rydberg energy scaled by the dielectric constant of the medium surrounding the ML and by the reduced effective electron-hole mass, whereas the ML polarizability is only accounted for by $δ$. This is justified by the analysis of experimental data on excitonic resonances, as extracted from magneto-optical measurements of a high-quality WSe$_2$ ML encaps…
First-Principles Investigation of Multimodal Toxic Gas Sensing in Carbon-Tuned hBN-Graphene Alloys: Chemiresistive, Work-Function, and Optical Responses
Stacking order in van der Waals materials determines the coupling between atomic layers and is therefore key to the materials' properties. By exploring different stacking orders, many novel physical phenomena have been realized in artificial vdW stacks. Recently, 2D ferroelectricity has been observed in zero-degree aligned hBN and graphene-hBN heterostructures, holding promise in a range of electronic applications. In those artificial stacks, however, the single domain size is limited by the stacking-angle misalignment to about 0.1 to 1 $μ$m, which is incompatible with most optical or optoelec…
Phase transitions of two-dimensional materials and their heterostructures enable many applications including electrochemical energy storage, catalysis, and memory; however, the nucleation pathways by which these transitions proceed remain underexplored, prohibiting engineering control for these applications. Here, we demonstrate that the lithium intercalation-induced 2H-1T' phase transition in MoS2 proceeds via nucleation of the 1T' phase at a heterointerface by monitoring the phase transition of MoS2/graphene and MoS2/hexagonal boron nitride (hBN) heterostructures with Raman spectroscopy in s…
We investigated experimentally the valley Zeeman splitting of excitonic peaks in the photoluminescence (PL) spectra of high-quality hBN/WS2/MoSe2/hBN heterostructures at near-zero twist angles under perpendicular magnetic fields up to 20 T. We identify two neutral exciton peaks in the PL spectra: the lower energy one exhibits a reduced g-factor relative to that of the higher energy peak, and much lower than the recently reported values for interlayer excitons in other van der Waals (vdW) heterostructures. We provide evidence that such a discernible g-factor stems from the spatial confinement o…
Using a novel approach to ultrafast resonant pump-probe spectroscopy we investigate the spectral shape and dynamics of absorption features related to the A exciton in an hBN/MoSe$_2$/hBN van der Waals heterostructure. While in a pure two-level system a pump-probe experiment measures the occupation or the polarization dynamics, depending on the time ordering of the pulse pair, in the transition metal dichalcogenide (TMD) system both quantities get thoroughly mixed by strong exciton-exciton interaction. We find that for short positive delays the spectral lines experience pronounced changes in th…
Twisted bilayer graphene (TBG) has taken the spotlight in the condensed matter community since the discovery of correlated phases at the so-called magic angle. Interestingly, the role of a substrate on the electronic properties of TBG has not been completely elucidated. Up to now, most of the theoretical works carried out in order to understand this effect have been done using continuum models. In this work, we have gone one step ahead and have studied heterostructures of TBG and hBN using an atomistic tight-binding model together with semi-classical molecular dynamics to take into account rel…
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 …
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…
Optical properties of atomically thin transition metal dichalcogenides are controlled by robust excitons characterized by a very large oscillator strength. Encapsulation of monolayers such as MoSe$_2$ in hexagonal boron nitride (hBN) yields narrow optical transitions approaching the homogenous exciton linewidth. We demonstrate that the exciton radiative rate in these van der Waals heterostructures can be tailored by a simple change of the hBN encapsulation layer thickness as a consequence of the Purcell effect. The time-resolved photoluminescence measurements together with cw reflectivity and …
Nanostructuring allows altering of the electronic and photonic properties of two-dimensional (2D) materials. The efficiency, flexibility, and convenience of top-down lithography processes are however compromised by nm-scale edge roughness and resolution variability issues, which especially affects the performance of 2D materials. Here we study how dry anisotropic etching of multilayer 2D materials with sulfur hexafluoride (SF6) may overcome some of these issues, showing results for hexagonal boron nitride (hBN), tungsten disulfide (WS2), tungsten diselenide (WSe2), molybdenum disulfide (MoS2),…
