We show that excitons and free carriers in K and K' valleys of transition metal dichalcogenide monolayers can be entangled with respect to their valley degree of freedom by absorbing linearly polarized single photons. This effect does not require any interaction between K and K' excitons in contrast to conventional mechanisms of entanglement that are mediated by coupling between quantum systems (e.g.~entanglement of photons in nonlinear optical interactions). The valley entanglement of excitons and free carriers can be verified by measuring the polarization of their photoluminescence or fluctuations of the photocurrent under an applied in-plane DC bias.
We propose a practical scheme to generate a pure valley current in monolayer transition metal dichalcogenides by one-photon absorption of linearly polarized light. We show that the pure valley current can be detected by either photoluminescence measurements or the ultrafast pump-probe technique. Our method, together with the previously demonstrated generation of valley polarization, opens up the exciting possibility of ultrafast optical-only manipulation of the valley index. The tilted field effect on the valley current in experiment is also discussed.
We study valley-dependent spin transport theoretically in monolayer transition-metal dichalcogenides in which a variety of spin and valley physics are expected because of spin-valley coupling. The results show that the spins are valley-selectively excited with appropriate carrier doping and valley polarized spin current (VPSC) is generated. The VPSC leads to the spin-current Hall effect, transverse spin accumulation originating from the Berry curvature in momentum space. The results indicate that spin excitations with spin-valley coupling lead to both valley and spin transport, which is promis…
We calculate the dispersion of spinor exciton-polaritons in a planar microcavity with its active region containing a single Transitional Metal Dichalcogenide (TMD) monolayer, taking into account excitonic and photonic spin-orbit coupling. We consider the radial propagation of polaritons in presence of disorder. We show that the reduction of the disorder scattering induced by the formation of polariton states allows to observe an optical Valley Hall effect, namely the coherent precession of the locked valley and polarization pseudospins leading to the formation of spatial valley-polarized domai…
The direct gap interband transitions in transition metal dichalcogenides monolayers are governed by chiral optical selection rules. Determined by laser helicity, optical transitions in either the $K^+$ or $K^-$ valley in momentum space are induced. Linearly polarized laser excitation prepares a coherent superposition of valley states. Here we demonstrate the control of the exciton valley coherence in monolayer WSe2 by tuning the applied magnetic field perpendicular to the monolayer plane. We show rotation of this coherent superposition of valley states by angles as large as 30 degrees in appli…
Although single-layer transition-metal dichalcogenides with novel valley functionalities are promising candidate to realize valleytronic devices, the essential understanding of valley depolarization mechanisms is still incomplete. Based on pump-probe experiments performed for MoSe2 and WSe2 monolayers and corroborating analysis from density functional calculations, we demonstrate that coherent phonons at the K-point of the Brillouin zone can effectively mediate the valley transfer of electron carriers. In the MoSe2 monolayer case, we identify this mode as the flexural acoustic ZA(K) mode, whic…
We develop a microscopic and atomistic theory of electron spin-based qubits in gated quantum dots in a single layer of transition metal dichalcogenides. The qubits are identified with two degenerate locked spin and valley states in a gated quantum dot. The two-qubit states are accurately described using a multi-million atom tight-binding model solved in wavevector space. The spin-valley locking and strong spin-orbit coupling result in two degenerate states, one of the qubit states being spin-down located at the $+K$ valley of the Brillouin zone, and the other state located at the $-K$ valley w…
Monolayer transition-metal dichalcogenides (TMDCs) have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. In these semiconducting materials, optically excited electron-hole pairs form tightly Coulomb-bound excitons with large binding energies. The selection rules for excitonic transitions allow for direct optical generation of a valley-polarized exciton population using resonant excitation. Here, we investigate the exciton valley dynamics in monolayers of three different TMDCs …
Lateral-hetero structures of atomic layered materials alter the electronic properties of pristine crystals and provide a possibility to produce useful monolayer materials. We reveal that metal-semiconductor-metal lateral-hetero junctions of $1H$-transition-metal dichalcogenides intrinsically possess conducting channels of electrons with spin-valley locking, e.g., gate electrode. We theoretically investigate the electronic structure and transport properties of the lateral-hetero junctions and show that the hetero-structure produces conducting channels through the $K$ and $K'$ valleys in the sem…
We reveal giant proximity-induced magnetism and valley-polarization effects in Janus Pt dichalcogenides (such as SPtSe), when bound to the Europium oxide (EuO) substrate. Using first-principles simulations, it is surprisingly found that the charge redistribution, resulting from proximity with EuO, leads to the formation of two K and K$^{'}$valleys in the conduction bands. Each of these valleys displays its own spin polarization and a specific spin-texture dictated by broken inversion and time-reversal symmetries, and valley-exchange and Rashba splittings as large as hundreds of meV. This provi…
Manipulating the valley degree of freedom to encode information for potential valleytronic devices has ignited a new direction in solid-state physics. A significant, fundamental challenge in the field of valleytronics is how to generate and regulate valley-polarized currents by practical ways. Here, we discover a new mechanism of producing valley polarization in a monolayer transition metal dichalcogenides superlattice, in which valley-resolved gaps are formed at the supercell Brillouin zone boundaries and centers due to the intervalley scattering. When the energy of the incident electron is i…
We consider theoretically staggered honeycomb lattices for photons which can be viewed as photonic analogs of transitional metal dichalcogenides (TMD) monolayers. We propose a simple realization of a photonic Quantum Valley Hall effect (QVHE) at the interface between two TMD analogs with opposite staggering on each side. This results in the formation of valley-polarized propagating modes whose existence relies on the difference between the valley Chern numbers, which is a $\mathbb{Z}_2$ topological invariant. We show that the magnitude of the photonic spin-orbit coupling based on the energy sp…
In this work, we predict the emergence of the valley Edelstein Effect (VEE), which is an electric-field-induced spin polarization effect, in gated monolayer transition metal dichalcogenides (MTMDs). We found an unconventional valley-dependent response in which the spin-polarization is parallel to the applied electric field with opposite spin-polarization generated by opposite valleys. This is in sharp contrast to the conventional Edelstein effect in which the induced spin-polarization is perpendicular to the applied electric field. We identify the origin of VEE as combined effects of conventio…
Quantum transport and spintronics regimes are studied in p- and n-doped atomic layers of hexagonal transition metal dichalcogenides (TMDCs), subject to the interplay between the valley structure and spin-orbit coupling. We find how spin relaxation of carriers depends on their areal density and show that it vanishes for holes near the band edge, leading to the density-independent spin diffusion length, and we develop a theory of weak localisation/antilocalisation, describing the crossovers between the orthogonal, double-unitary and symplectic regimes of quantum transport in TMDCs.
The performance limits of monolayer transition metal dichalcogenide transistors are examined with a ballistic MOSFET model. Using ab-initio theory, we calculate the band structures of two-dimensional (2D) transition metal dichalco-genide (MX2). We find the lattice structures of monolayer MX2 remain the same as the bulk MX2. Within the ballistic regime, the performances of monolayer MX2 transistors are better compared to the silicon transistors if thin high-κ gate insulator is used. This makes monolayer MX2 promising 2D materials for future nanoelectronic device applications.
We develop an analytical theory for edge states in monolayers of transition metal dichalcogenides based on a general boundary condition for a two-band ${\bf kp}$-Hamiltonian in case of uncoupled valleys. Taking into account {\it edge} spin-orbit interaction we reveal that edge states, in general, have linear dispersion that is determined by three real phenomenological parameters in the boundary condition. In absence of the edge spin-orbit interaction, edge states are described by a single real parameter whose sign determines whether their spectra intersect the bulk gap or not. In the former ca…
Spin and valley dependent anomalous Nernst effect are analyzed for monolayer MoS2 and other group-VI dichalcogenides. We find that pure spin and valley currents can be generated perpendicular to the applied thermal gradient in the plane of these two-dimensional materials. This effect provides a versatile platform for applications of spin caloritronics. A spin current purity factor is introduced to quantify this effect. When time reversal symmetry is violated, e.g. two-dimensional materials on an insulating magnetic substrate, a dip-peak feature appears for the total Nernst coefficient. For the…
In monolayer group-VI transition metal dichalcogenides (TMDC), charge carriers have spin and valley degrees of freedom, both associated with magnetic moments. On the other hand, the layer degree of freedom in multilayers is associated with electrical polarization. Here, we show that TMDC bilayers offer an unprecedented platform to realize a strong coupling between the spin, layer pseudospin, and valley degrees of freedom of holes. Such coupling not only gives rise to the spin Hall effect and spin circular dichroism in inversion symmetric bilayer, but also leads to a variety of magnetoelectric …
The rich phenomenology of plasmonic excitations in the dichalcogenides is analyzed as a function of doping. The many-body polarization, the dielectric response function and electron energy loss spectra are calculated using an ab initio based model involving material-realistic Coulomb interactions, band structure and spin-orbit coupling. Focusing on the representative case of MoS$_2$, a plethora of plasmon bands are observed, originating from scattering processes within and between the conduction or valence band valleys. We discuss the resulting square-root and linear collective modes, arising …
We report experimental evidences on selective occupation of the degenerate valleys in MoS2 monolayers by circularly polarized optical pumping. Over 30% valley polarization has been observed at K and K' valley via the polarization resolved luminescence spectra on pristine MoS2 monolayers. It demonstrates one viable way to generate and detect valley polarization towards the conceptual valleytronics applications with information carried by the valley index.
The band structure of many semiconducting monolayer transition metal dichalcogenides (TMDs) possesses two degenerate valleys, with equal and opposite Berry curvature. It has been predicted that, when illuminated with circularly polarized light, interband transitions generate an unbalanced non-equilibrium population of electrons and holes in these valleys, resulting in a finite Hall voltage at zero magnetic field when a current flows through the system. This is the so-called valley Hall effect that has recently been observed experimentally. Here, we show that this effect is mediated by photo-ge…
Preserving a high degree of valley polarization of excitons in photo-excited transition-metal dichalcogenide monolayers (TMD-MLs) is desirable for the valley-based photonic applications, but widely recognized as a hard task hindered by the intrinsic electron-hole exchange interaction. In this study, we present a comprehensive investigation of valley-polarized finite-momentum excitons in WSe$_2$-MLs over the entire Brillouin zone by solving the density-functional-theory(DFT)-based Bethe-Salpeter equation (BSE) under the guidance of symmetry analysis. We reveal that finite-momentum excitons are …
We present here results of atomistic theory of electrons confined by metallic gates in a single layer of transition metal dichalcogenides. The electronic states are described by the tight-binding model and computed using a computational box including up to million atoms with periodic boundary conditions and parabolic confining potential due to external gates embedded in it. With this methodology applied to MoS2, we find a twofold degenerate energy spectrum of electrons confined in the two non-equivalent K-valleys by the metallic gates as well as six-fold degenerate spectrum associated with Q-v…
Manipulating spin polarization of electrons in nonmagnetic semiconductors by means of electric fields or optical fields is an essential theme of the conceptual nonmagnetic semiconductor-based spintronics. Here we experimentally demonstrate a method of generating spin polarization in monolayer transition metal dichalcogenides (TMD) by the circularly polarized optical pumping. The fully spin-polarized photocurrent is achieved through the valley dependent optical selection rules and the spin-valley locking in monolayer WS2, and electrically detected by a lateral spin-valve structure with ferromag…
We study both the intrinsic and extrinsic spin Hall effect in spin-valley coupled monolayers of transition metal dichalcogenides. We find that whereas the skew-scattering contribution is suppressed by the large band gap, the side-jump contribution is comparable to the intrinsic one with opposite sign in the presence of scalar and magnetic scattering. Intervalley scattering tends to suppress the side-jump contribution due to the loss of coherence. By tuning the ratio of intra- to intervalley scattering, the spin Hall conductivity shows a sign change in hole-doped samples. Multiband effect in ot…
We investigate the electronic transport property of lateral heterojunctions of semiconducting and metallic transition-metal dichalcogenide monolayers, MoSe$_2$ and NbSe$_2$, respectively. We calculate the electronic transmission probability by using a multi-orbital tight-binding model based on the first-principles band structure. The transmission probability depends on the spin and valley degrees of freedom. This dependence qualitatively changes by the interface structure. The heterostructure with a zig-zag interface preserves the spin and the valley of electron in the transmission process. On…
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 …
We study the thermoelectric properties of monolayers of MoS$_{2}$ and other group-VI dichalcogenides under circularly polarized off-resonant light. Analytical expressions are derived for the Berry phase mediated magnetic moment, orbital magnetization, as well as thermal and Nernst conductivities. Tuning of the band gap by {\it off-resonant} light enhances the spin splitting in both the valence and conduction bands and, thus, leads to a dramatic improvement of the spin and valley thermoelectric properties.
We present low temperature magneto-photoluminescence experiments which demonstrate the brightening of dark excitons by an in-plane magnetic field $B$ applied to monolayers of different semiconducting transition metal dichalcogenides. For both WSe$_2$ and WS$_2$ monolayers, the dark exciton emission is observed at $\sim$50 meV below the bright exciton peak and displays a characteristic doublet structure which intensity is growing with $B^2$, while no magnetic field induced emission peaks appear for MoSe$_2$ monolayer. Our experiments also show that the MoS$_2$ monolayer has a dark exciton groun…
Electron valleys in transition-metal dichalcogenide monolayers drive novel physics and allow designing multifunctional architectures for applications. We propose to manipulate the electron valleys in these systems for spin/valley filter and valve devices through band engineering. Instead of the magnetic proximity effect that has been extensively used in previous studies, in our strategy, the electron valleys are directly coupled to the spin-polarized states of the two-dimensional ferromagnets. We find that this coupling results in a valley-selective gap opening due to the spin-momentum locking…
High degree of valley polarization of optically active excitons in transition-metal dichalcogenide monolayers (TMD-MLs) is vital in valley-based photonic applications but known to be likely spoiled by the intrinsic electron-hole exchange interactions. In this study, we present a theoretical investigation of the valley and optical properties of finite-momentum dark excitons in WSe$_2$-MLs by solving the density-functional-theory(DFT)-based Bethe-Salpeter equation (BSE) under the guidance of symmetry analysis. %We reveal that, in general, finite-momentum excitons are actually well immune from th…
We study the pseudo-spin of electron pair in superconducting transition-metal dichalcogenide monolayers and show that the pseudo-spin affects the electric transport property of lateral heterojunction of the superconducting and metallic monolayers. The pseudo-spins of two electrons forming a Cooper pair are parallel to each other unlike the real spins being anti-parallel. In the lateral heterojunction, the electronic transport with forming a Cooper pair, the Andreev reflection, is suppressed with the Fermi level crossing the valence band near the edge in the metallic monolayer. We numerically i…
We study the trion and biexciton in transition metal dichalcogenides monolayers within the framework of a nonrelativistic potential model using the method of hyperspherical harmonics (HH). We solve the three- and four-body Schrödinger equations with the Keldysh potential by expanding the wave functions of a trion and biexciton in terms of the antisymmetrized HH. Results of the calculations for the ground state energies are in good agreement with similar calculations for the Keldysh potential and in reasonable agreement with experimental measurements of trion and biexciton binding energies.
The valley pseudospin in monolayer transition metal dichalcogenides (TMDs) has been proposed as a new way to manipulate information in various optoelectronic devices. This relies on a large valley polarization that remains stable over long timescales (hundreds of ns). However, time resolved measurements report valley lifetimes of only a few ps. This has been attributed to mechanisms such as phonon-mediated inter-valley scattering and a precession of the valley psedospin through electron-hole exchange. Here we use transient spin grating to directly measure the valley depolarization lifetime in …
A rate equation model for the dark and bright excitons kinetics is proposed which explains the wide variation in the observed degree of circular polarization of the PL emission in different TMDs monolayers. Our work suggests that the dark exciton states play an important, and previously unsuspected role in determining the degree of polarization of the PL emission. A dark exciton ground state provides a robust reservoir for valley polarization, which tries to maintain a Boltzmann distribution of the bright exciton states in the same valley via the intra valley bright dark exciton scattering mec…
The newly developed two-dimensional layered materials provide perfect platform for valley-spintronics exploration. To determine the prospect of utilizing the valley degree of freedom, it is of great importance to directly detect and understand the valley dynamics in these materials. Here, the exciton valley dynamics in monolayer WSe$_2$ is investigated by the two-color pump-probe magneto-optical Kerr technique. By tuning the probe photon energy in resonance with the free excitons and trions, the valley relaxation time of different excitonic states in monolayer WSe$_2$ is determined. Valley rel…
We investigate valley dynamics associated with trions in monolayer tungsten diselenide (WSe2) using polarization resolved two-color pump-probe spectroscopy. When tuning the pump and probe energy across the trion resonance, distinct trion valley polarization dynamics are observed as a function of energy and attributed to the intra-valley and inter-valley trions in monolayer WSe2. We observe no decay of a near-unity valley polarization associated with the intra-valley trions during ~ 25 ps, while the valley polarization of the inter-valley trions exhibits a fast decay of ~ 4 ps. Furthermore, we …
We report experimental observation of 2s exciton radiative emission from monolayer tungsten diselenide, enabled by hexagonal boron nitride protected high-quality samples. The 2s luminescence is highly robust and persists up to 150K, offering a new quantum entity for manipulating the valley degree of freedom. Remarkably, the 2s exciton displays superior valley polarization and coherence than 1s under similar experimental conditions. This observation provides evidence that the Coulomb-exchange-interaction-driven valley-depolarization process, the Maialle-Silva-Sham mechanism, plays an important …
Monolayer transition metal dichalcogenids (TMDs) feature valley degree of freedom, giant spin-orbit coupling and spin-valley locking. These exotic natures stimulate efforts of exploring the potential applications in conceptual spintronics, valleytronics and quantum computing. Among all the exotic directions, a long lifetime of spin and/or valley polarization is critical. The present valley dynamics studies concentrate on the band edge excitons which predominates the optical response due to the enhanced Coulomb interaction in two dimensions. The valley lifetime of free carriers remains in ambig…
Intervalley scattering by atomic defects in monolayer transition metal dichalcogenides (TDMs; MX2) presents a serious obstacle for applications exploiting their unique valley-contrasting properties. Here, we show that the symmetry of the atomic defects can give rise to an unconventional protection mechanism against intervalley scattering in monolayer TMDs. The predicted defect-dependent selection rules for intervalley scattering can be verified via Fourier transform scanning tunneling spectroscopy (FT-STS), and provide a unique identification of, e.g., atomic vacancy defects (M vs X). Our find…
Monolayer transition metal dichalcogenides (TMDs) hold great promise for future information processing applications utilizing a combination of electron spin and valley pseudospin. This unique spin system has led to observation of the valley Zeeman effect in neutral and charged excitonic resonances under applied magnetic fields. However, reported values of the trion valley Zeeman splitting remain highly inconsistent across studies. Here, we utilize high quality hBN encapsulated monolayer WSe$_2$ to enable simultaneous measurement of both intervalley and intravalley trion photoluminescence. We f…
Monolayer films of transition metal dichalcogenides (in particular, MoS2, MoSe2, WS2, and WSe2) can be considered as ideal systems for the studies of high-temperature electron-hole liquids. The quasi-two-dimensional nature of electrons and holes ensures their stronger interaction as compared to that in bulk semiconductors. The screening of the Coulomb interaction in monolayer heterostructures is significantly reduced, since it is determined by the permittivities of the environment (e.g., vacuum and substrate), which are much lower than those characteristic of the films of transition metal dich…
We study the refraction effect of electronic wave in hole-doped lateral heterojunctions of metallic and semiconducting transition-metal dichalcogenide monolayers. This effect is theoretically investigated in 2$H$-type MoSe$_2$-NbS$_2$ and WSe$_2$-NbS$_2$ junctions by combining the first-principles calculation and the lattice Green's function method. We show that the electronic waves change the direction of motion at the interface and collimate the velocity along two different directions depending on the spin. We find that the transmission probability increases with the charge density and that …
We study the electronic spin relaxation effect in the hole-doped monolayer and bilayer transition-metal dichalcogenides in the presence of the crystal defects. We consider realistic models of the lattice vacancy and actually estimate the spin relaxation rate using the multi-orbital tight-binding model. In the monolayer, the spin-relaxation time is found to be extremely long compared to the momentum relaxation time, and this is attributed to the fact that the spin hybridization in the band structure is suppressed by the mirror reflection symmetry. The bilayer TMD has a much shorter spin relaxat…
We study the transport properties of monolayer MX2 (M = Mo, W; X = S, Se, Te) n- and p- channel metal-oxide-semiconductor field effect transistors (MOSFETs) using full-band ballistic non-equilibrium Green's function simulations with an atomistic tight-binding Hamiltonian with hopping potentials obtained from density functional theory. We discuss the subthreshold slope, drain-induced barrier lowering (DIBL), as well as gate-induced drain leakage (GIDL) for different monolayer MX2 MOSFETs. We also report the possibility of negative differential resistance behavior in the output characteristics o…
Localization of charge carriers in monolayers (MLs) of transition metal dichalcogenides (TMDs) dramatically increases spin and valley coherence times, and, by analogy with other systems, the role of the hyperfine interaction should enhance. We perform theoretical analysis of the intervalley hyperfine interaction in TMD MLs based on the group representation theory. We demonstrate, that the spin-valley locking leads to the helical structure of the in-plane hyperfine interaction. In the upper valence band the hyperfine interaction is shown to be of the Ising type, which can be used for fabricatio…
Transition metal dichalcogenide (TMD) monolayers are two-dimensional semiconductors with two valleys in their band structure that can be selectively addressed using circularly polarized light. Their photoluminescence spectrum is characterized by neutral and charged excitons (trions) that form a chemical equilibrium governed by the net charge density. Here, we use chemical doping to drive the conversion of excitons into trions in $\text{WS}_{2}$ monolayers at room temperature, and study the resulting valley polarization via photoluminescence measurements under valley-selective optical excitatio…
We derive a low-energy theory for edge states in transition metal dichalcogenide monolayers for a two-band $\bm{kp}$-Hamiltonian in case of uncoupled valleys. In the absence of spin-orbit interaction at the edge, these states possess a linear dispersion described by a single phenomenological parameter characterizing the edge structure. Depending on the sign of the parameter, the edge state spectrum can either cross the band gap or lie outside of it. In the first case, the presence of edge states leads to resonant enhancement of the second harmonic generation at frequencies about the half of th…
In the last few years, interest in monomolecular layers of transition metal dichalcogenides (TMDs) has been driven by their unusual electronic and optical properties, which are very attractive for designing functional elements of new generation nanoelectronics. Recently, experimental evidence has appeared for the formation of a high-temperature strongly bound electron-hole liquid (EHL) in TMD monolayers. Strong binding of charge carriers is due to a significant decrease in the screening of the Coulomb interaction in monolayer heterostructures. In this work, the gas--liquid phase transition in …
