Transition Metal Dichalcogenide Heterobilayers Research Articles

Room-temperature efficient and tunable interlayer exciton emissions in WS2/WSe2 heterobilayers at high generation rates.

Transition metal dichalcogenide (TMDC) heterobilayers (HBs) have been intensively investigated lately because they offer novel platforms for the exploration of interlayer excitons (IXs). However, the potentials of IXs in TMDC HBs have not been fully studied as efficient and tunable emitters for both photoluminescence (PL) and electroluminescence (EL) at room temperature (RT). Also, the efficiencies of the PL and EL of IXs have not been carefully quantified. In this work, we demonstrate that IX in WS2/WSe2 HBs could serve as promising emitters at high generation rates due to its immunity to efficiency roll-off. Furthermore, by applying gate voltages to balance the electron and hole concentrations and to reinforce the built-in electric fields, high PL quantum yield (QY) and EL external quantum efficiency (EQE) of ∼0.48% and ∼0.11% were achieved at RT, respectively, with generation rates exceeding 1021 cm-2·s-1, which confirms the capabilities of IXs as efficient NIR light emitters by surpassing most of the intralayer emissions from TMDCs.

Quantum Beats between Spin-Singlet and Spin-Triplet Interlayer Exciton Transitions in WSe2-MoSe2 Heterobilayers.

The long-lived interlayer excitons (IXs) of semiconducting transition metal dichalcogenide heterobilayers are prime candidates for developing various optoelectronic and valleytronic devices. Their photophysical properties, including fine structure, have been the focus of recent studies, and the presence of two spin states, namely, spin-singlet and spin-triplet, has been experimentally confirmed. However, the existence of the interaction between these states and their nature remains unknown to date. Here, we demonstrate the presence of coherent coupling between the spin-singlet and spin-triplet IXs of a WSe2-MoSe2 heterobilayer utilizing quantum beat spectroscopy via a home-built Michelson interferometer. As a clear signature of coherent coupling, the quantum beat signal has been observed for the first time between closely spaced transitions of IXs. The observed strong damping of the quantum beat signals with fast dephasing times of 270-400 fs indicates that fluctuations giving rise to inhomogeneous broadening in the photoluminescence emission of these states are uncorrelated.

Excitonic Mott insulator in a Bose-Fermi-Hubbard system of moiré WS2/WSe2 heterobilayer

Understanding the Hubbard model is crucial for investigating various quantum many-body states and its fermionic and bosonic versions have been largely realized separately. Recently, transition metal dichalcogenides heterobilayers have emerged as a promising platform for simulating the rich physics of the Hubbard model. In this work, we explore the interplay between fermionic and bosonic populations, using a WS2/WSe2 heterobilayer device that hosts this hybrid particle density. We independently tune the fermionic and bosonic populations by electronic doping and optical injection of electron-hole pairs, respectively. This enables us to form strongly interacting excitons that are manifested in a large energy gap in the photoluminescence spectrum. The incompressibility of excitons is further corroborated by observing a suppression of exciton diffusion with increasing pump intensity, as opposed to the expected behavior of a weakly interacting gas of bosons, suggesting the formation of a bosonic Mott insulator. We explain our observations using a two-band model including phase space filling. Our system provides a controllable approach to the exploration of quantum many-body effects in the generalized Bose-Fermi-Hubbard model.

Ultralow Auger-Assisted Interlayer Exciton Annihilation in WS2/WSe2 Moiré Heterobilayers.

Transition metal dichalcogenide (TMD) heterobilayers have emerged as a promising platform for exploring solid-state quantum simulators and many-body quantum phenomena. Their type II band alignment, combined with the moiré superlattice, inevitably leads to nontrivial exciton interactions and dynamics. Here, we unveil the distinct Auger annihilation processes for delocalized interlayer excitons in WS2/WSe2 moiré heterobilayers. By fitting the characteristic efficiency droop and bimolecular recombination rate, we quantitatively determine an ultralow Auger coefficient of 1.3 × 10-5 cm2 s-1, which is >100-fold smaller than that of excitons in TMD monolayers. In addition, we reveal selective exciton upconversion into the WSe2 layer, which highlights the significance of intralayer electron Coulomb interactions in dictating the microscopic scattering pathways. The distinct Auger processes arising from spatial electron-hole separation have important implications for TMD heterobilayers while endowing interlayer excitons and their strongly correlated states with unique layer degrees of freedom.

Enhancement of second-harmonic generation in a 64° stacked WSe2/WS2 heterobilayer with local strain

Transition metal dichalcogenides (TMDs) are actively studied in various fields of optics and optoelectronics, including nonlinear optics of second-harmonic generation (SHG). By stacking two different TMD materials to form a heterobilyaer, unique optical properties emerge, with stronger SHG at a twist angle of 0° between TMDs and weaker SHG at a twist angle of 60°. In this work, we demonstrate the enhancement of SHG in a heterobilayer consisting of WSe2 and WS2 monolayers stacked at a twist angle of 64.1°, using a nanoparticle to induce local strain. The interatomic spacing of the heterobilayer is deformed by the nanoparticle, breaking the inversion symmetry, resulting in a substantial increase in the SHG of the heterobilayer at room temperature. The SHG increases depending on the polarization of the pump laser: 15-fold for linear polarization, 9-fold for right-circular polarization, and up to 100-fold for left-circular polarization. In addition, the SHG enhanced in the heterobilayer with local strain satisfies the same chiral selection rule as in the unstrained TMD region, demonstrating that the chiral selection rule of SHG is insensitive to local strain. Our findings will increase the applicability of TMD heterobilayers in nonlinear optoelectronics and valleytronics.

Spatially-indirect and hybrid exciton–exciton interaction in MoS2 homobilayers

Interlayer excitons in transition-metal dichalcogenide (TMD) bilayers, alongside their interplay with direct excitonic species, are supposed to offer a pathway towards robust nonlinearity, enabling the exploration of many-body quantum effects. We present a theoretical investigation of interaction among various exciton species within these structures where Coulomb attraction and repulsion are subject to reduced screening. For a homobilayer MoS2, we examine both direct, spatially-indirect, and hybridised excitons, considering the effects of direct and exchange interaction of electrons and holes distributed across one or different layers. Similar physics arises in perfectly aligned twisted TMD heterobilayers which support the direct-to-indirect exciton hybridisation. Deriving the exciton–exciton interaction matrix elements, we unveil a distinct non-monotonic dependence of the interaction on transferred momentum, changing sign from repulsive to attractive even for ground-state excitons, and compare our results with existing calculations for monolayers. Our findings demonstrate that for large momenta involved in high-density effects (strongly correlated phases), the interaction is chiefly governed by the prevailing attractive exchange component. At the same time, at small momenta that are more relevant for rarefied systems, we find that the enhancement of the interaction constant for dipolar species compared to intralayer non-dipolar excitons may be hindered by the surrounding medium. We draw comparisons with existing experiments and discuss the implications of our findings on the collective effects in TMD-based systems of excitons and exciton-polaritons.

Evidence for ground state coherence in a two-dimensional Kondo lattice

Kondo lattices are ideal testbeds for the exploration of heavy-fermion quantum phases of matter. While our understanding of Kondo lattices has traditionally relied on complex bulk f-electron systems, transition metal dichalcogenide heterobilayers have recently emerged as simple, accessible and tunable 2D Kondo lattice platforms where, however, their ground state remains to be established. Here we present evidence of a coherent ground state in the 1T/1H-TaSe2 heterobilayer by means of scanning tunneling microscopy/spectroscopy at 340 mK. Our measurements reveal the existence of two symmetric electronic resonances around the Fermi energy, a hallmark of coherence in the spin lattice. Spectroscopic imaging locates both resonances at the central Ta atom of the charge density wave of the 1T phase, where the localized magnetic moment is held. Furthermore, the evolution of the electronic structure with the magnetic field reveals a non-linear increase of the energy separation between the electronic resonances. Aided by ab initio and auxiliary-fermion mean-field calculations, we demonstrate that this behavior is inconsistent with a fully screened Kondo lattice, and suggests a ground state with magnetic order mediated by conduction electrons. The manifestation of magnetic coherence in TMD-based 2D Kondo lattices enables the exploration of magnetic quantum criticality, Kondo breakdown transitions and unconventional superconductivity in the strict two-dimensional limit.

Localization and interaction of interlayer excitons in MoSe2/WSe2 heterobilayers

Transition metal dichalcogenide (TMD) heterobilayers provide a versatile platform to explore unique excitonic physics via the properties of the constituent TMDs and external stimuli. Interlayer excitons (IXs) can form in TMD heterobilayers as delocalized or localized states. However, the localization of IX in different types of potential traps, the emergence of biexcitons in the high-excitation regime, and the impact of potential traps on biexciton formation have remained elusive. In our work, we observe two types of potential traps in a MoSe2/WSe2 heterobilayer, which result in significantly different emission behavior of IXs at different temperatures. We identify the origin of these traps as localized defect states and the moiré potential of the TMD heterobilayer. Furthermore, with strong excitation intensity, a superlinear emission behavior indicates the emergence of interlayer biexcitons, whose formation peaks at a specific temperature. Our work elucidates the different excitation and temperature regimes required for the formation of both localized and delocalized IX and biexcitons and, thus, contributes to a better understanding and application of the rich exciton physics in TMD heterostructures.

Continuum model study of optical absorption by hybridized moiré excitons in transition metal dichalcogenide heterobilayers

Continuum model study of optical absorption by hybridized moiré excitons in transition metal dichalcogenide heterobilayers

Prolonged dephasing time of ensemble of moiré-trapped interlayer excitons in WSe2-MoSe2 heterobilayers

The moiré superlattices of transition metal dichalcogenide heterobilayers have a pronounced effect on the optical properties of interlayer excitons (IXs) and have been intensively studied in recent years. However, the impact of moiré potentials on the temporal coherence of the IXs has not yet been investigated in detail. Here, we systematically investigate the coherence properties of both the ensemble of delocalized and the ensemble of localized IXs trapped in moiré potentials of the hexagonal boron nitride encapsulated WSe2-MoSe2 heterostructures. Our low-temperature first-order correlation measurements show that prolonged T2 dephasing times with values up to 730 fs can be obtained from the ensemble of localized IXs under moderate pump powers. We observed up to almost a five-fold increase over the values we obtained from the delocalized IXs, while more than two-fold over the previously reported values of T2 ~ 300 fs from the delocalized IXs. The prolonged values of T2 dephasing times and narrow photoluminescence (PL) linewidths for the ensemble of moiré-trapped IXs compared to delocalized one indicate that dephasing mechanisms caused by exciton-low energy acoustic phonon and exciton-exciton scattering are significantly suppressed due to the presence of localization potentials. Our pump power-dependent T2 results show that ultra-long dephasing times can be expected if the dephasing time measurements are performed with the narrow photoluminescence emission line of a single moiré-trapped IX at a low pump power regime. The prolonged values of IX dephasing times would be critical for the applications of quantum information science and the development of two-dimensional material-based nanolasers.

Moiré Dirac fermions in transition metal dichalcogenides heterobilayers

Abstract Monolayer group-VIB transition metal dichalcogenides (TMDs) feature low-energy massive Dirac fermions, which have valley contrasting Berry curvature. This nontrivial local band topology gives rise to valley Hall transport and optical selection rules for interband transitions that open up new possibilities for valleytronics. However, the large bandgap in TMDs results in relatively small Berry curvature, leading to weak valley contrasting physics in practical experiments. Here, we show that Dirac fermions with tunable large Berry curvature can be engineered in moiré superlattice of TMD heterobilayers. These moiré Dirac fermions are created in a magnified honeycomb lattice with its sublattice degree of freedom formed by two local moiré potential minima. We show that applying an on-site potential can tune the moiré flat bands into helical ones. In short-period moiré superlattice, we find that the two moiré valleys become asymmetric, which results in a net spin Hall current. More interestingly, a circularly polarized light drives these moiré Dirac fermions into quantum anomalous Hall phase with chiral edge states. Our results open a new possibility to design the moiré-scale spin and valley physics using TMD moiré structures.

Observation and Modulation of High-Temperature Moiré-Locale Excitons in van der Waals Heterobilayers.

Transition metal dichalcogenide heterobilayers feature strong moiré potentials with multiple local minima, which can spatially trap interlayer excitons at different locations within one moiré unit cell (dubbed moiré locales). However, current studies mainly focus on moiré excitons trapped at a single moiré locale. Exploring interlayer excitons trapped at different moiré locales is highly desirable for building polarized light-emitter arrays and studying multiorbital correlated and topological physics. Here, via enhancing the interlayer coupling and engineering the heterointerface, we report the observation and modulation of high-temperature interlayer excitons trapped at separate moiré locales in WS2/WSe2 heterobilayers. These moiré-locale excitons are identified by two emission peaks with an energy separation of ∼60 meV, exhibiting opposite circular polarizations due to their distinct local stacking registries. With the increase of temperature, two momentum-indirect moiré-locale excitons are observed, which show a distinct strain dependence with the momentum-direct one. The emission of these moiré-locale excitons can be controlled via engineering the heterointerface with different phonon scattering, while their emission energy can be further modulated via strain engineering. Our reported highly tunable interlayer excitons provide important information on understanding moiré excitonic physics, with possible applications in building high-temperature excitonic devices.

Topological Superconductivity in Doped Magnetic Moiré Semiconductors.

We show that topological superconductivity may emerge upon doping of transition metal dichalcogenide heterobilayers above an integer-filling magnetic state of the topmost valence moiré band. The effective attraction between charge carriers is generated by an electric p-wave Feshbach resonance arising from interlayer excitonic physics and has a tunable strength, which may be large. Together with the low moiré carrier densities reachable by gating, this robust attraction enables access to the long-sought p-wave BEC-BCS transition. The topological protection arises from an emergent time reversal symmetry occurring when the magnetic order and long wavelength magnetic fluctuations do not couple different valleys. The resulting topological superconductor features helical Majorana edge modes, leading to half-integer quantized spin-thermal Hall conductivity and to charge currents induced by circularly polarized light or other time-reversal symmetry-breaking fields.

Intrinsic Control of Interlayer Exciton Generation in Van der Waals Materials via Janus Layers

We demonstrate the possibility of engineering the optical properties of transition metal dichalcogenide heterobilayers when one of the constitutive layers has a Janus structure. We investigate different MoS2@Janus layer combinations using first-principles methods including excitons and exciton-phonon coupling. The direction of the intrinsic electric field from the Janus layer modifies the electronic band alignments and, consequently, the energy separation between dark interlayer exciton states and bright in-plane excitons. We find that in-plane lattice vibrations strongly couple the two states, so that exciton-phonon scattering may be a viable generation mechanism for interlayer excitons upon light absorption. In particular, in the case of MoS2@WSSe, the energy separation of the low-lying interlayer exciton from the in-plane exciton is resonant with the transverse optical phonon modes (40 meV). We thus identify this heterobilayer as a prime candidate for efficient generation of charge-separated electron-hole pairs.

Tunable interlayer excitons and switchable interlayer trions via dynamic near-field cavity

Emerging photo-induced excitonic processes in transition metal dichalcogenide (TMD) heterobilayers, e.g., interplay of intra- and inter-layer excitons and conversion of excitons to trions, allow new opportunities for ultrathin hybrid photonic devices. However, with the associated large degree of spatial heterogeneity, understanding and controlling their complex competing interactions in TMD heterobilayers at the nanoscale remains a challenge. Here, we present an all-round dynamic control of interlayer-excitons and -trions in a WSe2/Mo0.5 W0.5 Se2 heterobilayer using multifunctional tip-enhanced photoluminescence (TEPL) spectroscopy with <20 nm spatial resolution. Specifically, we demonstrate the bandgap tunable interlayer excitons and the dynamic interconversion between interlayer-trions and -excitons, through the combinational tip-induced engineering of GPa-scale pressure and plasmonic hot electron injection, with simultaneous spectroscopic TEPL measurements. This unique nano-opto-electro-mechanical control approach provides new strategies for developing versatile nano-excitonic/trionic devices using TMD heterobilayers.

Berry curvature, spin Hall effect, and nonlinear optical response in moiré transition metal dichalcogenide heterobilayers

Recently, topological flat bands and the spin Hall effect have been experimentally observed in AB-stacked ${\mathrm{MoTe}}_{2}/{\mathrm{WSe}}_{2}$ heterostructures. In this paper, we systematically study the Berry curvature effects in moir\'e transition metal dichalcogenide (TMD) heterobilayers. We point out that the moir\'e potential of the remote conduction bands would induce a sizable periodic pseudomagnetic field (PMF) on the valence band. This periodic PMF creates net Berry curvature flux in each valley of the moir\'e Brillouin zone. The combination of the effect of the Berry curvature and the spin-valley locking can induce the spin Hall effect being observed in the experiment. Interestingly, the valley-contrasting Berry curvature distribution generated by the PMF can be probed through shift currents, which are dc currents induced by linearly polarized light through nonlinear responses. Our work sheds light on the novel quantum phenomena induced by Berry curvature in moir\'e TMD heterobilayers.

Negative Valley Polarization of the Intralayer Exciton via One-Step Growth of H-Type Heterobilayer WS2/MoS2

Vertical type II van der Waals heterobilayers of transition metal dichalcogenides (TMDs) have attracted wide attention due to their distinctive features mostly arising from the emergence of intriguing electronic structures that include moiré-related phenomena. Owing to strong spin-orbit coupling under a noncentrosymmetric environment, TMD heterobilayers host nonequivalent +K and -K valleys of contrasting Berry curvatures, which can be optically controlled by the helicity of optical excitation. The corresponding valley selection rules are well established by not only intralayer excitons but also interlayer excitons. Quite intriguingly, here, we experimentally demonstrate that unusual valley switching can be achieved using the lowest-lying intralayer excitons in H-type heterobilayer WS2/MoS2 prepared by one-step growth. This TMD combination provides an ideal case for interlayer coupling with an almost perfect lattice match, thereby also in the momentum space between +K and -K valleys in the H-type heterostructure. The underlying valley-switching mechanism can be understood by bright-to-dark conversion of initially created electrons in the valley of WS2, followed by interlayer charge transfer to the opposite valley in MoS2. Our suggested model is also confirmed by the absence of valley switching when the lowest-lying excitons in MoS2 are directly generated in the heterobilayer. In contrast to the H-type case, we show that no valley switching is observed from R-type heterobilayers prepared by the same method, where interlayer charge transfer does not occur between the opposite valleys. We compare the case with the series of valley polarization data from other heterobilayer combinations obtained under different excitation energies and temperatures. Our valley switching mechanism can be utilized for valley manipulation by controlling the excitation photon energy together with the photon helicity in valleytronic devices derived from H-type TMD heterobilayers.

Magnetic-field-induced Wigner crystallization of charged interlayer excitons in van der Waals heterostructures

Ever since its inception, coherent excited states of semiconductors have been the focus of semiconductor materials research to evolve into a vibrant field of low-dimensional solid-state physics. The field is gaining new momentum these days due to emerging transdimensional semiconductors such as van der Waals bound layers of transition metal dichalcogenides (TMDs) of controlled thickness. Here, we develop the theory of magnetic-field-induced Wigner crystallization for charged interlayer excitons (CIE) discovered recently in TMD heterobilayers. We derive the ratio of the potential interaction energy to the kinetic energy for the many-particle CIE system in the perpendicular magnetostatic field of an arbitrary strength and predict the crystallization effect in the strong field regime. We show that magnetic-field-induced Wigner crystallization and melting of CIEs can be observed in magneto-photoluminescence experiments with TMD bilayers of systematically varied electron-hole doping concentrations. Our results advance the capabilities of this new generation of transdimensional quantum materials.

Melting of generalized Wigner crystals in transition metal dichalcogenide heterobilayer Moiré systems

Moiré superlattice systems such as transition metal dichalcogenide heterobilayers have garnered significant recent interest due to their promising utility as tunable solid state simulators. Recent experiments on a WSe2/WS2 heterobilayer detected incompressible charge ordered states that one can view as generalized Wigner crystals. The tunability of the transition metal dichalcogenide heterobilayer Moiré system presents an opportunity to study the rich set of possible phases upon melting these charge-ordered states. Here we use Monte Carlo simulations to study these intermediate phases in between incompressible charge-ordered states in the strong coupling limit. We find two distinct stripe solid states to be each preceded by distinct types of nematic states. In particular, we discover microscopic mechanisms that stabilize each of the nematic states, whose order parameter transforms as the two-dimensional E representation of the Moiré lattice point group. Our results provide a testable experimental prediction of where both types of nematic occur, and elucidate the microscopic mechanism driving their formation.

Spin-Polarized Charge Separation in a Photoexcited Transition Metal Dichalcogenide Heterobilayer at Room Temperature

Spin-Polarized Charge Separation in a Photoexcited Transition Metal Dichalcogenide Heterobilayer at Room Temperature