We study the dark excitons at the interface of sharp lateral heterostructure of two-dimensional transition metal dichalcogenides. By introducing a low-energy effective Hamiltonian model, we find the energy dispersion relation of exciton and show how it depends on the onsite energy of composed materials and their spin-orbit coupling strengths. It is shown that the effect of geometrical structure of interface, as a deformation gauge field (pseudo-spin-orbit coupling), should be considered in calculating the binding energy of exciton. By discretization of real-space version of the dispersion relation on a triangular lattice, we show that the binding energy of exciton depends on its distance from the interface line. For exciton near the interface the binding energy is equal to 0.36 eV, while for the exciton enough far from the interface it is equal to 0.26 eV. Also, it has been shown that for zigzag interface the binding energy increases by 0.34 meV in comparison with the armchair interface due to the pseudo-spin-orbit interaction (gauge filed). The results can be used for designing the two-dimensional lateral heterostructure based optoelectronic devices and improving their characteristics.
We investigate theoretically the electronic structure of graphene and boron nitride (BN) lateral heterostructures, which were fabricated in recent experiments. The first-principles density functional calculation demonstrates that a huge intrinsic transverse electric field can be induced in the graphene nanoribbon region, and depends sensitively on the edge configuration of the lateral heterostructure. The polarized electric field originates from the charge mismatch at the BN-graphene interfaces. This huge electric field can open a significant bang gap in graphene nanoribbon, and lead to fully …
Indirect excitons (IXs) in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by a high binding energy making them stable at room temperature and giving the opportunity for exploring fundamental phenomena in excitonic systems and developing excitonic devices operational at high temperatures. We present the observation of IXs at room temperature in van der Waals TMD heterostructures based on monolayers of MoS$_2$ separated by atomically thin hexagonal boron nitride. The IXs realized in the TMD heterostructure have lifetimes orders of magnitude longer than lif…
Theory of exciton fine structure in semiconductor quantum dots and its dependence on quantum dot anisotropy and external lateral electric field is presented. The effective exciton Hamiltonian including long range electron-hole exchange interaction is derived within the k*p effective mass approximation (EMA). The exchange matrix elements of the Hamiltonian are expressed explicitly in terms of electron and hole envelope functions. The matrix element responsible for the "bright" exciton splitting is identified and analyzed. An excitonic fine structure for a model quantum dot with quasi- two-dimen…
We study the response of exciton complexes in semiconductor quantum rings to vertical electric fields, using path integral quantum Monte Carlo simulations. The interaction of a vertical applied field and the piezoelectric fields of the ring with strongly-correlated excitonic complexes switches excitons between two different lateral locations within the ring. This control should be observable through polarizability and dipole measurements, and, for biexcitons, an energy shift beyond the normal Stark shift.
The predicted formation of moire superlattices leading to confined excitonic states in heterostructures formed by stacking two lattice mismatched transition metal dichalcogenide (TMD) monolayers was recently experimentally confirmed. Such periodic potential in TMD heterostructure functions as a diffusion barrier that affects the energy transport and dynamics of interlayer excitons (electron and hole spatially concentrated in different monolayers). Understanding the transport of excitons under such condition is essential to establish the material system as a next generation device platform. In …
We report an experimental study of excitons in a double quantum well van der Waals heterostructure made of atomically thin layers of \Mo* and hexagonal boron nitride (hBN). The emission of neutral and charged excitons is controlled by gate voltage, temperature, and both the helicity and the power of optical excitation.
Long lifetimes of spatially indirect excitons (IXs), also known as interlayer excitons, make possible long-range IX propagation. Van der Waals heterostructures composed of atomically thin layers of transition-metal dichalcogenides (TMDs) give an opportunity to realize excitons with high binding energies and provide a materials platform for the realization of both excitonic quantum phenomena and excitonic devices. Propagation of IXs in TMD heterostructures is intensively studied. However, in spite of long IX lifetimes, orders of magnitude longer than lifetimes of spatially direct excitons (DXs)…
Indirect excitons (IXs), also known as interlayer excitons, can form the medium for excitonic devices whose operation is based on controlled propagation of excitons. A proof of principle for excitonic devices was demonstrated in GaAs heterostructures where the operation of excitonic devices is limited to low temperatures. IXs in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by high binding energies making IXs robust at room temperature and offering an opportunity to create excitonic devices operating at high temperatures suitable for applications. Howev…
We study transport of indirect excitons in GaAs/AlGaAs coupled quantum wells in linear lattices created by laterally modulated gate voltage. The localization-delocalization transition (LDT) for transport across the lattice was observed with reducing lattice amplitude or increasing exciton density. The exciton interaction energy at the transition is close to the lattice amplitude. These results are consistent with the model, which attributes the LDT to the interaction-induced percolation of the exciton gas through the external potential. We also discuss applications of the lattice potentials fo…
Based on \emph{ab initio} theoretical calculations of the optical spectra of vertical heterostructures of MoSe$_2$ (or MoS$_2$) and WSe$_2$ sheets, we reveal two spin-orbit-split Rydberg series of excitonic states below the \textsl{A} excitons of MoSe$_2$ and WSe$_2$ with a significant binding energy on the order of 250\,meV for the first excitons in the series. At the same time, we predict crystalographically aligned MoSe$_2$/WSe$_2$ heterostructures to exhibit an indirect fundamental band gap. Due to the type-II nature of the MoSe$_2$/WSe$_2$ heterostructure, the indirect transition and the …
We investigate excitons in stacked transition metal dichalcogenide (TMDC) layers under perpendicularly applied electric field, herein MoSe$_2$/WSe$_2$ van der Waals heterostructures. Band structures are obtained with density functional theory calculations, along with the electron and hole wave functions in conduction and valence bands, respectively. Although the type-II nature of the heterostructure leads to fully charge separated inter-layer excitons, charge carriers distribution among the layers is shown to be easily tunable by external field. Our results show that moderate values of electri…
We study the interface exciton at lateral type II heterojunctions of monolayer transition metal dichalcogenides (TMDs), where the electron and hole prefer to stay at complementary sides of the junction. We find that the 1D interface exciton has giant binding energy in the same order as 2D excitons in pristine monolayer TMDs although the effective radius (electron-hole seperation) of interface exciton is much larger than that of 2D excitons. The binding energy, exciton radius and optical dipole strongly depends on the band offset at the junction. The inter-valley coupling induced by the electro…
Previously, graphene nanoribbons set in lateral heterostructures with hexagonal boron nitride were predicted to support topologically protected states at low energy. We investigate how robust the transport properties of these states are against lattice disorder. We find that forms of disorder that do not couple the two valleys of the zigzag graphene nanoribbon do not impact the transport properties at low bias, indicating that these lateral heterostructures are very promising candidates for chip-scale conducting interconnects. Forms of disorder that do couple the two valleys, such as vacancies…
The fine structure of the neutral exciton in a single self assembled InGaAs quantum dot is investigated under the effect of a lateral electric field. Stark shifts up to 1.5 meV, an increase in linewidth, and a decrease in photoluminescence intensity were observed due to the electric field. We show that the lateral electric field strongly affects the exciton fine structure splitting due to active manipulation of the single particle wave-functions. Remarkably, the splitting can be tuned over large values and through zero.
We demonstrate the localisation of quantum well excitons in a periodic array of linear traps using photoluminescence experiments. The excitonic traps are induced by applying spatially alternating external voltages via interdigitated metal gates. The localisation originates from the periodical modulation of the strength of the quantum-confined Stark effect in the plane of the quantum well. In our experiments, the trap depth is easily tuned by the voltages applied to the interdigitated gates. Furthermore, we find that a perpendicular magnetic field reduces the exciton diffusion length. In short-…
Stacking monolayers of transition metal dichalcogenides into a heterostructure with a finite twist-angle gives rise to artificial moiré superlattices with a tunable periodicity. As a consequence, excitons experience a periodic potential, which can be exploited to tailor optoelectronic properties of these materials. While recent experimental studies have confirmed twist-angle dependent optical spectra, the microscopic origin of moiré exciton resonances has not been fully clarified yet. Here, we combine first principle calculations with the excitonic density matrix formalism to study transitions…
Monolayer (ML) transition metal dichalcogenides (TMDs) integrated in optical microcavities host exciton-polaritons as a hallmark of the strong light-matter coupling regime. Analogous concepts for hybrid light-matter systems employing spatially indirect excitons with a permanent electric dipole moment in heterobilayer (HBL) crystals promise realizations of exciton-polariton gases and condensates with immanent dipolar interactions. Here, we identify optical signatures of spatially indirect momentum-bright and momentum-dark interlayer excitons in vertical MoSe$_2$-WSe$_2$ heterostructures and imp…
Exciton binding energies of hundreds of meV and strong light absorption in the optical frequency range make transition metal dichalcogenides (TMDs) promising for novel optoelectronic nanodevices. In particular, atomically thin TMDs can be stacked to heterostructures enabling the design of new materials with tailored properties. The strong Coulomb interaction gives rise to interlayer excitons, where electrons and holes are spatially separated in different layers. In this work, we reveal the microscopic processes behind the formation, thermalization and decay of these fundamentally interesting a…
We report on the observation of terahertz radiation induced photogalvanic currents in semiconductor heterostructures with one-dimensional lateral periodic potential. The potential is produced by etching a grating into the sample surface. The electric current response is well described by phenomenological theory including both the circular and linear photogalvanic effects. Experimental data demonstrate that the inversion asymmetry of the periodic lateral pattern can be varied by means of electron beam lithography to produce classical lateral ratchets. A novel microscopical mechanism for the pol…
In heterostructures consisting of different transition-metal dichalcogenide monolayers, a staggered band alignment can occur, leading to rapid charge separation of optically generated electron-hole pairs into opposite monolayers. These spatially separated electron-hole pairs are Coulomb-coupled and form interlayer excitons. Here, we study these interlayer excitons in a heterostructure consisting of MoSe$_2$ and WSe$_2$ monolayers using photoluminescence spectroscopy. We observe a non-trivial temperature dependence of the linewidth and the peak energy of the interlayer exciton, including an unu…
Two-dimensional semiconductors have emerged as a new class of materials for nanophotonics for their strong exciton-photon interaction and flexibility for engineering and integration. Taking advantage of these properties, we engineer an efficient lasing medium based on dipolar interlayer excitons, in rotationally aligned atomically thin heterostructures. Lasing is measured from a transition metal dichalcogenide hetero-bilayer integrated in a silicon nitride grating resonator. A sharp increase in the spatial coherence of the emission was observed across the lasing threshold. The work establishes…
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…
Semiconductor heterostructures are backbones for solid state based optoelectronic devices. Recent advances in assembly techniques for van der Waals heterostructures has enabled the band engineering of semiconductor heterojunctions for atomically thin optoelectronic devices. In two-dimensional heterostructures with type II band alignment, interlayer excitons, where Coulomb-bound electrons and holes are confined to opposite layers, have shown promising properties for novel excitonic devices, including a large binding energy, micron-scale in-plane drift-diffusion, and long population and valley p…
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…
Atomically precise lateral heterojunctions based on transition metal dichalcogenides provide a new platform for exploring exciton Mott transition in one-dimension. To investigate the intrinsically non-equilibrium Mott transition, we employed ultrafast microscopy with ~ 200 fs temporal resolution to image the transport of different exciton phases in a type II WSe2-WS1.16Se0.84 lateral heterostructure. These measurements visualized the extremely rapid expansion of a highly non-equilibrium electron-hole (e-h) plasma phase with a Fermi velocity up to 3.2*10^6 cm*s-1. An abrupt first-order exciton …
Excitons in semiconductors, bound pairs of excited electrons and holes, can form the basis for new classes of quantum optoelectronic devices. A van der Waals heterostructure built from atomically thin semiconducting transition metal dichalcogenides (TMDs) enables the formation of excitons from electrons and holes in distinct layers, producing interlayer excitons with large binding energy and a long lifetime. Employing heterostructures of monolayer TMDs, we realize optical and electrical generation of long-lived neutral and charged interlayer excitons. We demonstrate the transport of neutral in…
Long-lived interlayer excitons with distinct spin-valley physics in van der Waals heterostructures based on transition metal dichalcogenides make them promising for information processing in next-generation devices. While the emission characteristics of interlayer excitons in different types of hetero stacks have been extensively studied, the manipulation of these excitons required to alter the valley-state or tune the emission energy and intensity is still lacking. Here, we demonstrate such control over interlayer excitons in MoSe2/WSe2 heterostructures. The encapsulation of our stack with h-…
Excitons are composite bosons that can feature spin singlet and triplet states. In usual semiconductors, without an additional spin-flip mechanism, triplet excitons are extremely inefficient optical emitters. Large spin-orbit coupling in transition metal dichalcogenides (TMDs) couples circularly polarized light to excitons with selective valley and spin. Here, we demonstrate electrically controlled brightening of spin-triplet interlayer excitons in a MoSe$_2$/WSe$_2$ TMD van der Waals (vdW) heterostructure. The atomic registry of vdW layers in TMD heterostructures provides a quasi-angular mome…
Indirect excitons (IX) in semiconductor heterostructures are bosons, which can cool below the temperature of quantum degeneracy and can be effectively controlled by voltage and light. IX quantum Bose gases and IX devices were explored in GaAs heterostructures where an IX range of existence is limited to low temperatures due to low IX binding energies. IXs in van der Waals transition-metal dichalcogenide (TMD) heterostructures are characterized by large binding energies giving the opportunity for exploring excitonic quantum gases and for creating excitonic devices at high temperatures. TMD hete…
Van der Waals heterostructures constitute a platform for investigating intriguing many-body quantum phenomena. In particular, transition-metal dichalcogenide (TMD) hetero-bilayers host long-lived interlayer excitons which exhibit permanent out-of-plane dipole moments. Here, we develop a microscopic theory for interlayer exciton-exciton interactions including both the dipolar nature of interlayer excitons as well as their fermionic substructure, which gives rise to an attractive fermionic exchange. We find that these interactions contribute to a drift force resulting in highly non-linear excito…
Moiré superlattices provide a powerful tool to engineer novel quantum phenomena in two-dimensional (2D) heterostructures, where the interactions between the atomically thin layers qualitatively change the electronic band structure of the superlattice. For example, mini-Dirac points, tunable Mott insulator states, and the Hofstadter butterfly can emerge in different types of graphene/boron nitride moiré superlattices, while correlated insulating states and superconductivity have been reported in twisted bilayer graphene moiré superlattices. In addition to their dramatic effects on the single pa…
We investigated excitonic absorptions in GaAs/AlAs/GaAs single barrier heterostructure using both photocapacitance and photocurrent spectroscopies at room temperature. Photocapacitance spectra show well defined resonance peak of indirect excitons formed around the Gamma-AlAs barrier. Unlike DC-photocurrent spectra, frequency dependent photocapacitance spectra interestingly red shift, sharpen up and then decrease with increasing tunneling at higher biases. Such dissimilarities clearly point out that different exciton dynamics govern these two spectral measurements. We also argue why such quantu…
Monolayers of transition metal dichalcogenides (TMDCs) feature exceptional optical properties that are dominated by excitons, tightly bound electron-hole pairs. Forming van der Waals heterostructures by deterministically stacking individual monolayers allows to tune various properties via choice of materials and relative orientation of the layers. In these structures, a new type of exciton emerges, where electron and hole are spatially separated. These interlayer excitons allow exploration of many-body quantum phenomena and are ideally suited for valleytronic applications. Mostly, a basic mode…
(Ga,In)As/GaAs/Ga(As,Sb) multi-quantum well heterostructures have been investigated using continuous wave and time-resolved photoluminescence spectroscopy at various temperatures. A complex interplay was observed between the excitonic type-II transitions with electrons in the (Ga,In)As well and holes in the Ga(As,Sb) well and the type-I excitons in the (Ga,In)As and Ga(As,Sb) wells. The type-II luminescence exhibits a strongly non-exponential temporal behavior below a critical temperature of Tc = 70K. The transients were analyzed in the framework of a rate-equation model. It was found that the…
Elimination of the acoustoelectric domain and increasing of the emission intensity by means of shunting the lateral current in the InGaAs/GaAs heterostructures
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…
Reduced electron screening in two-dimension plays a fundamental role in determining exciton properties, which dictates optoelectronic and photonic device performances. Considering the explicit electron-hole interaction within the $GW-$Bethe-Salpeter formalism, we first study the excitonic properties of pristine phosphorene and investigate the effects of strain and impurity coverage. The calculations reveal strongly bound exciton in these systems with anisotropic spatial delocalization. Further, we present a simplified hydrogenic model with anisotropic exciton mass and effective electron screen…
In van der Waals (vdW) heterostructures formed by stacking two monolayer semiconductors, lattice mismatch or rotational misalignment introduces an in-plane moiré superlattice. While it is widely recognized that a moiré superlattice can modulate the electronic band structure and lead to novel transport properties including unconventional superconductivity and insulating behavior driven by correlations, its influence on optical properties has not been investigated experimentally. We present spectroscopic evidence that interlayer excitons are confined by the moiré potential in a high-quality MoSe…
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…
Stacking atomic monolayers of semiconducting transition metal dichalcogenides (TMDs) has emerged as an effective way to engineer their properties. In principle, the staggered band alignment of TMD heterostructures should result in the formation of inter-layer excitons with long lifetimes and robust valley polarization. However, these features have been observed simultaneously only in MoSe$_2$/WSe$_2$ heterostructures. Here we report on the observation of long lived inter-layer exciton emission in a MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructure. The inter-layer nature of the o…
A supersolid, a counter-intuitive quantum state in which a rigid lattice of particles flows without resistance, has to date not been unambiguously realised. Here we reveal a supersolid ground state of excitons in a double-layer semiconductor heterostructure over a wide range of layer separations outside the focus of recent experiments. This supersolid conforms to the original Chester supersolid with one exciton per supersolid site, as distinct from the alternative version reported in cold-atom systems of a periodic modulation of the superfluid density. We provide the phase diagram augmented by…
High-Energy Interlayer Exciton Ensembles in MoSe$_2$/WSe$_2$ Heterostructures by Laguerre-Gaussian Excitation
Walter Schottky Institute and Physics Department, TU Munich（慕尼黑工业大学沃尔特·肖特基研究所与物理系）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Institute of Physics, University of Münster（明斯特大学物理研究所）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国立材料研究所材料纳米架构研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国立材料研究所电子与光学材料研究中心）
Throughout the years, strongly correlated coherent states of excitons have been the subject of intense theoretical and experimental studies. This topic has recently boomed due to new emerging quantum materials such as van der Waals (vdW) bound atomically thin layers of transition metal dichalcogenides (TMDs). We analyze the collective properties of charged interlayer excitons observed recently in bilayer TMD heterostructures. We predict new strongly correlated phases - crystal and Wigner crystal - that can be selectively realized with TMD bilayers of properly chosen electron-hole effective mas…
In this work, we study the spin polarization in the $MoS(Se)_{2}-WS(Se)_{2}$ Transition metal dichalcogenide heterostructures by using the non-equilibrium Green's function (NEGF) method and a three-band tight-binding model near the edges of the first Brillouin zone. Although it has been shown that the structures have no significant spin polarization in a specific range of energy of electrons, by applying a transverse electric field in the sheet of the metal atoms, shedding light on the sample, and under a small bias voltage, a significant spin polarization in the structure could be created. Be…
