Recent techniques have allowed transition metal dichalcogenides (TMD) monolayers to be grown and adequately characterised. Of particular interest, their nonlinear optical response presents many promising opportunities for future nanophotonic devices and technology. The dispersion of the carriers is trigonally-warped, leading to an anisotropic Fermi surface for low-lying states. In this paper, the effects of such a deformation on the nonlinear harmonic generation are studied by considering a tight-binding model expanded up to third order in $\mathbf{k} \cdot \mathbf{p}$. By solving exactly the free-carrier dynamics of the carriers when interacting with intense and ultrashort pulses of light, we predict the photogenerated current in a nonperturbative way and study its harmonic composition. We find frequency and amplitude modulation of the nonlinear current in quadratic and cubic models. Furthermore, we demonstrate anisotropy-induced modulation of the intensity of higher-order harmonics and the existence of harmonic crossovers, depending on the incident light polarisation. The methodology presented in this paper may be applied to any general effective two-band model and offer a pathway to identify signatures of electronic features in optical output.
The intrinsic orbital magnetization of a TMD monolayer is usually calculated for a plane unbounded system without mentioning the geometrical shape of samples and boundary conditions (BCs) for electron wave functions. The method of calculations includes allowing for the Berry curvature contribution also in the case when the system is described by the two-band minimal model [9]. In the present paper, we show that the geometrical and topological properties of the specimen, as well as the BCs, play an important role in the problem of magnetization even for a macroscopic specimen.
Monolayers of transition metal dichalcogenides (TMDs) in the 2H structural phase have been recently classified as higher-order topological insulators (HOTI), protected by $C_3$ rotation symmetry. In addition, theoretical calculations show an orbital Hall plateau in the insulating gap of TMDs, characterized by an orbital Chern number. We explore the correlation between these two phenomena in TMD monolayers in two structural phases: the noncentrosymmetric 2H and the centrosymmetric 1T. Using density functional theory, we confirm the characteristics of 2H-TMDs and reveal that 1T-TMDs are identifi…
When considering transition-metal dichalcogenides (TMDCs) in van der Waals (vdW) heterostructures for periodic ab-initio calculations, usually, lattice mismatch is present, and the TMDC needs to be strained. In this study we provide a systematic assessment of biaxial strain effects on the orbital, spin-orbit, and optical properties of the monolayer TMDCs using ab-initio calculations. We complement our analysis with a minimal tight-binding Hamiltonian that captures the low-energy bands of the TMDCs around K and K' valleys. We find characteristic trends of the orbital and spin-orbit parameters a…
We propose a scheme for the spatial exciton energy control and exciton routing in a transition metal dichalcogenide (TMD) monolayer which lies on a quantum paraelectric substrate. It relies on the ultrasensitive response of the substrate dielectric permittivity to temperature changes, allowing for spatially inhomogeneous screening of Coulomb interaction in a monolayer. As an example, we consider the heterostructure of TMD and strontium titanate oxide SrTiO$_3$, where large dielectric screening can be attained. We study the impact of substrate temperature on the characteristic electronic featur…
Understanding the ultrafast coupling and relaxation mechanisms between valleys in transition metal dichalcogenide semiconductors is of crucial interest for future valleytronic devices. Recent ultrafast pump-probe experiments showed an unintuitive significant bleaching at the excitonic $B$ transition after optical excitation of the energetically lower excitonic $A$ transition. Here, we present a possible microscopic explanation for this surprising effect. It is based on the joint action of exchange coupling and phonon-mediated thermalization into dark exciton states and does not involve a popul…
We theoretically investigate the corrections of exciton binding energy in monolayer transition metal dichalcogenides (TMDs) due to the exciton-optical phonon coupling in the Fr$\ddot{o}$hlich interaction model by using the linear operator combined Lee-Low-Pines variational method. We not only consider the excitons couple with the intrinsic longitudinal optical (LO) phonon modes, but also the surface optical phonon modes that induced by the polar substrates underneath the TMDs. We find that exciton binding energies are corrected in a large scale due to these exciton-optical phonon couplings. We…
The excitonic states of transition metal dichacolgenide (TMD) monolayers are heavily influenced by their external dielectric environment based on the substrate used. In this work, various wide bandgap dielectric materials, namely hexagonal boron nitride (\textit{h}-BN) and amorphous silicon nitride (Si$_3$N$_4$), under different configurations as support or encapsulation material for WS$_2$ monolayers are investigated to disentangle the factors contributing to inhomogeneous broadening of exciton absorption lines in TMDs using electron energy loss spectroscopy (EELS) in a scanning transmission …
In atomically thin two-dimensional semiconductors such as transition metal dichalcogenides (TMDs), controlling the density and type of defects promises to be an effective approach for engineering light-matter interactions. We demonstrate that electron-beam irradiation is a simple tool for selectively introducing defect-bound exciton states associated with chalcogen vacancies in TMDs. Our first-principles calculations and time-resolved spectroscopy measurements of monolayer WSe2 reveal that these defect-bound excitons exhibit exceptional optical properties including a recombination lifetime app…
We theoretically study the interaction of an ultrafast intense linearly polarized optical pulse with monolayers of transition metal dichalcogenides (TMDCs). Such a strong pulse redistributes electrons between the bands and generates femtosecond currents during the pulse. Due to the large bandwidth of the incident pulse, this process is completely off-resonant. While in TMDCs the time-reversal symmetry is conserved, the inversion symmetry is broken and these monolayers have the axial symmetry along armchair direction but not along the zigzag one. Therefore, the pulse polarized along the asymmet…
Atomic disorder is a common limiting factor for the low-temperature mobility in monolayer transition-metal dichalcogenides (TMDs; MX2). Here, we study the effect of often occurring atomic vacancies on carrier scattering and transport in p- and n-type monolayer MoS2. Due to charge trapping in vacancy-induced in-gap states, both neutral and charged vacancies resembling, respectively, short-range and combined short-range and long-range Coulomb scatterers, must be considered. Using the T-matrix formalism, we demonstrate a strong renormalization of the Born description of short-range scattering, ma…
Suspended monolayer transition metal-dichalcogenides (TMD) are membranes that combine ultra-low mass and exceptional optical properties, making them intriguing materials for opto-mechanical applications. However, the low measured quality factor of TMD resonators has been a roadblock so far. Here, we report an ultrasensitive optical readout of monolayer TMD resonators that allows us to reveal their mechanical properties at cryogenic temperatures. We find that the quality factor of monolayer WSe2 resonators greatly increases below room temperature, reaching values as high as 1.6E^4 at liquid nit…
Monolayers (MLs) of transition metal dichalcogenides (TMDs) such as WSe2 and MoSe2 can be placed by dry stamping directly on broadband dielectric resonators, which have the ability to enhance the spontaneous emission rate and brightness of solid-state emitters at room temperature. We show strongly enhanced emission and directivity modifications in room temperature photoluminescence mapping experiments. By varying TMD material (WSe2 versus MoSe2) transferred on silicon nanoresonators with various designs (planarized versus non-planarized), we experimentally separate the different physical mecha…
We study theoretically the Coulomb interaction between excitons in transition metal dichalcogenide (TMD) monolayers. We calculate direct and exchange interaction for both ground and excited states of excitons. The screening of the Coulomb interaction, specific to monolayer structures, leads to the unique behavior of the exciton-exciton scattering for excited states, characterized by the non-monotonic dependence of the interaction as function of the transferred momentum. We find that the nontrivial screening enables the description of TMD exciton interaction strength by approximate formula whic…
Strong Coulomb correlations together with multi-valley electronic bands in the presence of spin-orbit interaction and possible new optoelectronic applications are at the heart of studies of the rich physics of excitons in semiconductor structures made of monolayers of transition metal dichalcogenides (TMD). In intrinsic TMD monolayers the basic, intravalley excitons are formed by a hole from the top of the valence band and an electron either from the lower or upper spin-orbit-split conduction band subbands: one of these excitons is optically active, the second one is "dark", although possibly …
We study a system of a transition metal dichalcogenide (TMD) monolayer placed in an optical resonator, where strong light-matter coupling between excitons and photons is achieved. We present quantitative theory of the nonlinear optical response for exciton-polaritons for the case of doped TMD monolayer, and analyze in detail two sources of nonlinearity. The first nonlinear response contribution stems from the Coulomb exchange interaction between excitons. The second contribution comes from the reduction of Rabi splitting that originates from phase space filling at increased exciton concentrati…
Uniform Narrow Excitonic Spectrum in Large-Area Suspended WSe2 Monolayers
NTT Basic Research Laboratories, NTT, Inc.（NTT基础研究所）；Department of Materials Science, Graduate School of Engineering, Tohoku University（东北大学大学院工学研究科材料科学系）；Center for Science and Innovation in Spintronics, Tohoku University（东北大学自旋电子学科学与创新中心）；Quantum Materials and Applications Research Center, National Institutes for Quantum Science and Technology（量子科学技术研究院量子材料与应用研究中心）
In this work, we present a comprehensive theoretical and computational investigation of exciton fine structures of WSe$_2$-monolayers, one of the best known two-dimensional (2D) transition-metal dichalcogenides (TMD's), in various dielectric-layer environments by solving the first-principles-based Bethe-Salpeter equation. While the physical and electronic properties of atomically thin nano-materials are normally sensitive to the variation of surrounding environment, our studies reveal that the influence of dielectric environment on the exciton fine structures of TMD-ML's is surprisingly limite…
The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observ…
Two-dimensional transition metal dichalcogenide (2D-TMD) monolayers, which reveal remarkable semiconductor properties, are the subject of active experimental research.Recently it has been shown experimentally that quantum yield in MoS2 and WSe2 monoatomic layers can reach values close to unity when electrostatic doping makes them intrinsic semiconductors. However, the available theoretical description does not give an understanding of the physical mechanisms underlying in the gate voltage control of quantum yield.This work is an attempt to propose a consistent semi-phenomenological theory of p…
The optical spectra of transition metal dichalcogenide (TMDC) monolayers are dominated by excitons and trions. Here we establish the dependences of these optical transitions on disorder from hyperspectral imaging of h-BN encapsulated monolayer MoSe2. While both exciton and trion energies vary spatially, these two quantities are almost perfectly correlated, with spatial variation in the trion binding energy of only ~0.18 meV. In contrast, variation in the energy splitting between the two lowest energy exciton states is one order of magnitude larger at ~1.7 meV. Statistical analysis and theoreti…
Monolayer transition metal dichalcogenides (TMDs) exhibit high nonlinear optical (NLO) susceptibilities. Experiments on MoS$_2$ have indeed revealed very large second-order ($χ^{(2)}$) and third-order ($χ^{(3)}$) optical susceptibilities. However, third harmonic generation results of other layered TMDs has not been reported. Furthermore, the reported $χ^{(2)}$ and $χ^{(3)}$ of MoS$_2$ vary by several orders of magnitude, and a reliable quantitative comparison of optical nonlinearities across different TMDs has remained elusive. Here, we investigate second- and third-harmonic generation, and th…
In order to fully exploit the potential of transition metal dichalcogenide monolayers (TMD-MLs), the well-controlled creation of atomically sharp lateral heterojunctions within these materials is highly desirable. A promising approach to create such heterojunctions is the local modulation of the electronic structure of an intrinsic TMD-ML via dielectric screening induced by its surrounding materials. For the realization of this non-invasive approach, an in-depth understanding of such dielectric effects is required. We report on the modulations of excitonic transitions in TMD-MLs through the ef…
Atomically thin transition metal dichalcogenide crystals (TMDCs) have extraordinary optical properties that make them attractive for future optoelectronic applications. Integration of TMDCs into practical all-dielectric heterostructures hinges on the ability to passivate and protect them against necessary fabrication steps on large scales. Despite its limited scalability, encapsulation of TMDCs in hexagonal boron nitride (hBN) currently has no viable alternative for achieving high performance of the final device. Here, we show that the novel, ultrathin Ga$_2$O$_3$ glass is an ideal centimeter-…
Atomically thin materials, like semiconducting transition metal dichalcogenides (S-TMDs), are highly sensitive to the environment. This opens up an opportunity to externally control their properties by changing their surroundings. We investigate the effect of several metallic substrates on the optical properties of MoSe$_2$ monolayer (ML) deposited on top of them with photoluminescence and reflectance contrast techniques. The optical spectra of MoSe$_{2}$ MLs deposited on Pt, Au, Mo and Zr have distinctive metal-related lineshapes. In particular, a substantial variation in the intensity ratio …
It is shown that potential barriers in bilayer graphene (BLG) and monolayer transition metal dichalcogenides (TMDs) can split a valley unpolarized incident current into reflected and transmitted currents with opposite valley polarization. Valley asymmetric transmission inevitably occurs because of the low symmetry of the total Hamiltonian and when total external reflection occurs the transmission is 100% valley polarized in BLG and 100% spin and valley polarized in TMDs, except for exponentially small corrections. By adjusting the potential, 100% polarization can be obtained regardless of the …
Using time-resolved Kerr rotation, we measure the spin/valley dynamics of resident electrons and holes in single charge-tunable monolayers of the archetypal transition-metal dichalcogenide (TMD) semiconductor WSe2. In the n-type regime, we observe long (70 ns) polarization relaxation of electrons that is sensitive to in-plane magnetic fields $B_y$, indicating spin relaxation. In marked contrast, extraordinarily long (2 microsecond) polarization relaxation of holes is revealed in the p-type regime, that is unaffected by $B_y$, directly confirming long-standing expectations of strong spin-valley…
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 strong light-matter interaction in monolayer transition metal dichalcogenides (TMDs) is promising for nanoscale optoelectronics with their direct band gap nature and the ultra-fast radiative decay of the strongly bound excitons these materials host. However, the impeded amount of light absorption imposed by the ultra-thin nature of the monolayers impairs their viability in photonic applications. Using a layered heterostructure of a monolayer TMD stacked on top of strongly absorbing, non-luminescent, multi-layer SnSe2, we show that both single-photon and two-photon luminescence from the TMD…
Despite its extremely weak intrinsic spin-orbit coupling (SOC), graphene has been shown to acquire considerable SOC by proximity coupling with exfoliated transition metal dichalcogenides (TMDs). Here we demonstrate strong induced Rashba SOC in graphene that is proximity coupled to a monolayer TMD film, MoS2 or WSe2, grown by chemical vapor deposition with drastically different Fermi level positions. Graphene/TMD heterostructures are fabricated with a pickup-transfer technique utilizing hexagonal boron nitride, which serves as a flat template to promote intimate contact and therefore a strong i…
Charged excitons (trions) are essential for the optical spectra in low dimensional doped monolayers (ML) of transitional metal dichalcogenides (TMDC). Using a direct diagonalization of the three-body Hamiltonian, we explore the low-lying trion states in four types of TMDC MLs. We show that the trions fine structure results from the interplay between the spin-valley fine structure of the single-particle bands and the exchange interaction between the composing particles. We demonstrate that by variations of the doping and dielectric environment, trion energy fine structure can be tuned, leading …
Atomically thin transition metal dichalcogenides (TMDs) have distinct opto-electronic properties including enhanced luminescence and high on-off current ratios, which can be further modulated by making more complex TMD heterostructures. However, resolution limits of conventional optical methods do not allow for direct optical-structural correlation measurements in these materials, particularly of buried interfaces in TMD heterostructures. Here we use, for the first time, electron beam induced cathodoluminescence in a scanning transmission electron microscope (CL-STEM) to measure optical proper…
Chiral interaction between light and two-dimensional transition metal dichalcogenides (2D-TMDs) has recently drawn enormous scientific attention. The optical selection rules of these atomically thin semiconductors allow the attribution of a pseudospin to the TMDs' valleys, which can be coherently manipulated for information processing using polarized light. The interaction of TMDs with circularly and linearly polarized light creates the valley polarization and coherence, respectively. With a full Stokes polarization analysis of light emitted from WS2 monolayer flakes, we conclusively confirm t…
The electronic and optoelectronic properties of two dimensional materials have been extensively explored in graphene and layered transition metal dichalcogenides (TMDs). Spintronics in these two-dimensional materials could provide novel opportunities for future electronics, for example, efficient generation of spin current, which should enable the efficient manipulation of magnetic elements. So far, the quantitative determination of charge current induced spin current and spin-orbit torques (SOTs) on the magnetic layer adjacent to two-dimensional materials is still lacking. Here, we report a l…
Monolayer transition metal dichalcogenides (TMD) have numerous potential applications in ultrathin electronics and photonics. The exposure of TMD based devices to light generates photo-carriers resulting in an enhanced conductivity, which can be effectively used, e.g., in photodetectors. If the photo-enhanced conductivity persists after removal of the irradiation, the effect is known as persistent photoconductivity (PPC). Here we show that ultraviolet light (wavelength = 365 nm) exposure induces an extremely long-living giant PPC (GPPC) in monolayer MoS2 (ML-MoS2) field-effect transistors (FET…
The monolithic integration of electronics and photonics has attracted enormous attention due to its potential applications. However, the realization of such hybrid circuits has remained a challenge because it requires optical communication at nanometer scales. A major challenge to this integration is the identification of a suitable material. After discussing the material aspect of the challenge, we identified atomically thin transition metal dichalcogenides (TMDs) as a perfect material platform to implement the circuit. The selection of TMDs is based on their very distinct property: monolayer…
We propose and analyze a mechanism for inducing spin Hall currents in ordinary (1H phase) monolayer transition metal dichalcogenides (TMDs) due to the nonlinear process of optical rectification. The photo-induced spin current is proportional to the light intensity, and originates from the intrinsic spin-orbit coupling in TMDs. The spin current spectrum is strongly influenced by electron-hole interactions, i.e. excitonic effects, analogous to the optical absorption. Remarkably, excitons change the temperature dependence of the induced spin current, to the point that the current direction can ev…
Tunneling light-emitting devices (LEDs) based on transition metal dichalcogenides (TMDs) and other 2D materials are a new platform for on-chip optoelectronic integration. Some of the physical processes underlying this LED architecture are not fully understood, especially the emission at photon energies higher than the applied electrostatic potential, so-called overbias emission. Here we report overbias emission for potentials that are near half of the optical bandgap energy in TMD-based tunneling LEDs. We show that this emission is not thermal in nature, but consistent with exciton generation …
Photoluminescence (PL) of transition metal dichalcogenide (TMD) monolayers is strongly influenced by the dielectric environment. The defect states present in the substrate induces uncontrollable doping in the TMD monolayer and thereby modifies the PL spectra. There have been enormous efforts to tune and overcome the effect of inevitable subtract defects in PL spectra, but a proper understanding and a convenient way are still lacking. Here, we systematically studied the effect of surface defects by gradually increasing the separation between WS2 monolayer and substrate. Hence, we could precisel…
Transition metal dichalcogenides (TMDs) are an exciting family of 2D materials; a member of this family, MoS$_2$, became the first measured monolayer semiconductor. In this article, a generalized phenomenological continuum model for the optical vibrations of the monolayer TMDs valid in the long-wavelength limit is developed. Non-polar oscillations involve differential equations for the phonon displacement vector that describe phonon dispersion up to a quadratic approximation. On the other hand, the polar modes satisfy coupled differential equations for the displacement vectors and the inner el…
The rich optical properties of transition metal dichalcogenide monolayers (TMD-MLs) render these materials promising candidates for the design of new optoelectronic devices. Despite the large number of excitonic complexes in TMD-MLs, the main focus has been put on optically bright neutral excitons. Spin-forbidden dark excitonic complexes have been addressed for basic science purposes, but not for applications. We report on spin-forbidden dark excitonic complexes in ML WSe$_2$ as an ideal system for the facile generation of radially polarized light beams. Furthermore, the spatially resolved pol…
Excitons in monolayer transition-metal-dichalcogenides (TMDs) dominate their optical response and exhibit strong light-matter interactions with lifetime-limited emission. While various approaches have been applied to enhance light-exciton interactions in TMDs, the achieved strength have been far below unity, and a complete picture of its underlying physical mechanisms and fundamental limits has not been provided. Here, we introduce a TMD-based van der Waals heterostructure cavity that provides near-unity excitonic absorption, and emission of excitonic complexes that are observed at ultra-low e…
Atomically thin semiconductors made from transition metal dichalcogenides (TMDs) are model systems for investigations of strong light-matter interactions and applications in nanophotonics, opto-electronics and valley-tronics. However, the photoluminescence spectra of TMD monolayers display a large number of features that are particularly challenging to decipher. On a practical level, monochromatic TMD-based emitters would be beneficial for low-dimensional devices but this challenge is yet to be resolved. Here, we show that graphene, directly stacked onto TMD monolayers enables single and narro…
