Heterobilayers consisting of MoSe$_2$ and WSe$_2$ monolayers can host optically bright interlayer excitons with intriguing properties such as ultralong lifetimes and pronounced circular polarization of their photoluminescence due to valley polarization, which can be induced by circularly polarized excitation or applied magnetic fields. Here, we report on the observation of an intrinsic valley-magnetophonon resonance for localized interlayer excitons promoted by invervalley hole scattering. It leads to a resonant increase of the photoluminescence polarization degree at the same field of 24.2 Tesla for H-type and R-type stacking configurations despite their vastly different excitonic energy splittings. As a microscopic mechanism of the hole intervalley scattering we identify the scattering with chiral TA phonons of MoSe$_2$ between excitonic states mixed by the long-range electron hole exchange interaction.
A double peak structure in the magneto-phonon resonance (MPR) spectrum of uniaxial strained graphene, under crossed electric and magnetic fields, is predicted. We focus on the $Γ$ point optical phonon modes coupled to the inter-Landau level transitions $0 \leftrightarrows \pm 1$ where MPR is expected to be more pronounced at high magnetic field. We derive the frequency shifts and the broadenings of the longitudinal (LO) and transverse (TO) optical phonon modes taking into account the effect of the strain modified electronic spectrum on the electron-phonon coupling. We show that the MPR lines a…
Interlayer valley excitons in bilayer MoS2 feature concurrently large oscillator strength and long lifetime, and hence represent an advantageous scenario for valleytronic applications. However, control of valley pseudospin of interlayer excitons in pristine bilayer MoS2, which lies at the heart of valleytronics, has remained elusive. Here we report the observation of highly circularly polarized photoluminescence from interlayer excitons of bilayer MoS2 with both optical and magnetic addressability. Under excitation of circularly polarized light near exciton resonance, interlayer excitons of bi…
We show that, because of the inevitable twist and lattice mismatch in heterobilayers of transition metal dichalcogenides, interlayer excitons have six-fold degenerate light cones anomalously located at finite velocities on the parabolic energy dispersion. The photon emissions at each light cone are elliptically polarized, with major axis locked to the direction of exciton velocity, and helicity specified by the valley indices of the electron and the hole. These finite-velocity light cones allow unprecedented possibilities to optically inject valley polarization and valley current, and the obse…
Heterostructures comprising different monolayer semiconductors provide a new system for fundamental science and device technologies, such as in the emerging field of valleytronics. Here, we realize valley-specific interlayer excitons in monolayer WSe2-MoSe2 vertical heterostructures. We create interlayer exciton spin-valley polarization by circularly polarized optical pumping and determine a valley lifetime of 40 nanoseconds. This long-lived polarization enables the visualization of the expansion of a valley-polarized exciton cloud over several microns. The spatial pattern of the polarization …
Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and tripl…
For monolayer transition metal chalcogenides (TMDs), electrons and excitons in different valleys can be driven to opposite directions by the Berry curvature, serving as a valley-dependent effective magnetic field. In addition to monolayer TMDs, Van der Waals heterostructures provide an attractive platform for emerging valley physics and devices with superior physics properties. Interlayer excitons in TMD heterostructures have a long valley lifetime as compared to monolayer intralayer excitons. Here we report an interlayer exciton valley polarization and valley Hall effect in MoS2/WSe2 in room …
Photoluminescence (PL) from excitons serves as a powerful tool to characterize the optoelectronic property and band structure of semiconductors, especially for atomically thin 2D transition metal chalcogenide (TMD) materials. However, PL quenches quickly when the thickness of TMD material increases from monolayer to few-layers, due to the change from direct to indirect band transition. Here we show that PL can be recovered by engineering multilayer heterostructures, with the band transition reserved to be direct type. We report emission from layer engineered interlayer excitons from these mult…
A twisted graphene bilayer exhibits a triangular Moiré pattern in the local stacking, that smoothly alternates between the three basic types AA', AB' and BA'. Under an interlayer bias U, the latter two types develop a spectral gap, characterised by opposite valley Chern numbers. We show that for large enough Moiré periods and bias, these regions become depleted electronically, and topologically protected helical modes appear at their boundaries. This gives rise to a delocalised topological network of the Chalker-Coddington type, composed of valley current vortices. This network can be tailored…
Two-dimensional semiconductors feature valleytronics phenomena due to locking of the spin and momentum valley of the electrons. However, the valley polarization is intrinsically limited in monolayer crystals by the fast intervalley electron-hole exchange. Hetero-bilayer crystals have been shown to have a longer exciton lifetime and valley depolarization time. But the reported valley polarization was low; the valley selection rules and mechanisms of valley depolarization remains controversial. Here, we report singlet and brightened triplet interlayer excitons both with over 80% valley polarizat…
Moiré superlattices provide a powerful way to engineer properties of electrons and excitons in two-dimensional van der Waals heterostructures. The moiré effect can be especially strong for interlayer excitons, where electrons and holes reside in different layers and can be addressed separately. In particular, it was recently proposed that the moiré superlattice potential not only localizes interlayer exciton states at different superlattice positions, but also hosts an emerging moiré quasi-angular momentum (QAM) that periodically switches the optical selection rules for interlayer excitons at …
The interlayer couplings in commensurate and incommensurate bilayer structures of transition metal dichalcogenides are investigated with perturbative treatment. The interlayer coupling in \pm K valleys can be decomposed into a series of hopping terms with distinct phase factors. In H-type and R-type commensurate bilayers, the interference between the three main terms leads to a sensitive dependence of the interlayer coupling strength on the translation. The magnitudes of the main hopping terms are found to some dozen of meV by fitting to the ab initio results. The interlayer couplings in Γvall…
The recent proposal of using an anisotropic vacuum for generating valley coherence in transition metal dichalcogenide (TMDC) monolayers has expanded the potential of such valley degrees of freedom for applications in valleytronics. In this work, we open up a completely new regime, inaccessible with monolayer TMDCs, of spontaneously generated valley coherence in interlayer excitons in commensurate TMDC bilayer heterostructures. Using the peculiar out of plane polarization of interlayer excitons in conjunction with an in-plane anisotropic electromagnetic vacuum, we show that a much larger region…
Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moiré interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe$_2$-WSe$_2$ stacks as representative realizations of twisted van der Waals bilayer and trilayer heterostructures, we observe contrasting optical signatures and interpret them in the theoretical framework of interlay…
Van der Waals heterostructures formed by two different monolayer semiconductors have emerged as a promising platform for new optoelectronic and spin/valleytronic applications. In addition to its atomically thin nature, a two-dimensional semiconductor heterostructure is distinct from its three-dimensional counterparts due to the unique coupled spin-valley physics of its constituent monolayers. Here, we report the direct observation that an optically generated spin-valley polarization in one monolayer can be transferred between layers of a two-dimensional MoSe2-WSe2 heterostructure. Using nondeg…
In van der Waals heterostructures (HS) consisting of stacked MoSe$_2$ and WSe$_2$ monolayers, optically bright interlayer excitons (ILE) can be observed when the constituent layers are crystallographically aligned. The symmetry of the monolayers allows for two different types of alignment, in which the momentum-direct interlayer transitions are either valley-conserving (R-type alignment) or changing the valley index (H-type anti-alignment). Here, we study the valley polarization dynamics of ILE in magnetic fields up to 30~Tesla by time-resolved photoluminescence (PL). For all ILE types, we fin…
Excitons in monolayer semiconductors have large optical transition dipole for strong coupling with light field. Interlayer excitons in heterobilayers, with layer separation of electron and hole components, feature large electric dipole that enables strong coupling with electric field and exciton-exciton interaction, at the cost that the optical dipole is substantially quenched (by several orders of magnitude). In this letter, we demonstrate the ability to create a new class of excitons in transition metal dichalcogenide (TMD) hetero- and homo-bilayers that combines the advantages of monolayer-…
Degenerate extrema in the energy dispersion of charge carriers in solids, also referred to as valleys, can be regarded as a binary quantum degree of freedom, which can potentially be used to implement valleytronic concepts in van der Waals heterostructures based on transition metal dichalcogenides. Using magneto-photoluminescence spectroscopy, we achieve a deeper insight into the valley polarization and depolarization mechanisms of interlayer excitons formed across a MoS$_2$/MoSe$_2$/MoS$_2$ heterostructure. We account for the non-trivial behavior of the valley polarization as a function of th…
Photo-induced charge separation in transition metal dichalcogenide heterobilayers is being explored for moiré excitons, spin-valley polarization, and quantum phases of excitons/electrons. While different momentum spaces may be critically involved in charge separation dynamics, little is known directly from experiments. Here we determine momentum-resolved electron dynamics in the WS2/MoS2 heterobilayer using time and angle resolved photoemission spectroscopy (TR-ARPES). Upon photoexcitation in the K valleys, we detect electrons in M/2, M, and Q valleys/points on time scales as short as ~70 fs, …
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-…
Manipulating and reserving the valley pseudospin of excitons is one core aim in the two-dimensional transition metal dichalcogenides (TMDs). However, due to the strong electron-hole exchange and spin-orbit coupling interactions, the exciton recombination lifetime is subject to picosecond timescale intrinsically, and the valley polarization is hardly modulated by a moderate magnetic field. It is fortunate that interlayer and defect-localized excitons promise to overcome these difficulties by suppressing the above interactions. Here we clearly reveal that the valley polarization can be reversed …
We describe the effects of the crossing of the exciton levels in moire quantum dots in external magnetic field. We demonstrate that the unpolarized light can create significant dynamic valley polarization of interlayer excitons in the conditions where the Zeeman energy is much smaller than the thermal energy. The angular momentum is gained by the excitons from the nuclear spin fluctuations. In the $n$-type moire quantum dots for the typical experimental parameters, the unpolarized light can lead to the complete valley polarization of the resident electrons.
We investigate the optical properties of spin-triplet interlayer excitons in heterobilayer transition metal dichalcogenides in comparison with the spin-singlet ones. Surprisingly, the optical transition dipole of the spin-triplet exciton is found to be in the same order of magnitude to that of the spin-singlet exciton, in sharp contrast to the monolayer excitons where the spin triplet species is considered as dark compared to the singlet. Unlike the monolayer excitons whose spin-conserved (spin-flip) transition dipole can only couple to light of in-plane (out-of-plane) polarization, such restr…
Multiple magnetic states, valley electronics, and topological phase transitions in two-dimensional Janus XYZH (X = Sc, Y, La, Y = Cl, Br, I, and Z = S, Se, Te): From monolayers to bilayers
The creation of moiré patterns in crystalline solids is a powerful approach to manipulate their electronic properties, which are fundamentally influenced by periodic potential landscapes. In 2D materials, a moiré pattern with a superlattice potential can form by vertically stacking two layered materials with a twist and/or finite lattice constant difference. This unique approach has led to emergent electronic phenomena, including the fractal quantum Hall effect, tunable Mott insulators, and unconventional superconductivity. Furthermore, theory predicts intriguing effects on optical excitations…
We introduce the concept of valley-layer coupling (VLC) in two-dimensional materials, where the low-energy electronic states in the emergent valleys have valley-contrasted layer polarization such that each state is spatially localized on the top or bottom super-layer. The VLC enables a direct coupling between valley and gate electric field, opening a new route towards electrically controlled valleytronics. We analyze the symmetry requirements for the system to host VLC, demonstrate our idea via first-principles calculations and model analysis of a concrete 2D material example, and show that an…
In Bernal stacked bilayer graphene interlayer coupling significantly affects the electronic bandstructure compared to monolayer graphene. Here we present magnetotransport experiments on high-quality $n$-doped bilayer MoS$_{2}$. By measuring the evolution of the Landau levels as a function of electron density and applied magnetic field we are able to investigate the occupation of conduction band states, the interlayer coupling in pristine bilayer MoS$_{2}$, and how these effects are governed by electron-electron interactions. We find that the two layers of the bilayer MoS$_{2}$ behave as two in…
Moiré interlayer exciton in transition metal dichalcogenide heterobilayer features a permanent electric dipole that enables the electrostatic control of its flow, and optical dipole that is spatially varying in the moiré landscape. We show the hybridization of moiré interlayer exciton with photons in a planar 2D cavity leads to two types of moiré polaritons that exhibit distinct forms of topological transport phenomena including the spin/valley Hall and polarization Hall effects, which feature remarkable electrical tunability through the control of exciton-cavity detuning by the interlayer bia…
Monolayers of semiconducting transition metal dichalcogenides exhibit intriguing fundamental physics of strongly coupled spin and valley degrees of freedom for charge carriers. While the possibility of exploiting these properties for information processing stimulated concerted research activities towards the concept of valleytronics , maintaining control over spin-valley polarization proved challenging in individual monolayers. A promising alternative route explores type II band alignment in artificial van der Waals heterostructures. The resulting formation of interlayer excitons combines the …
Valley polarization of moiré interlayer exciton complexes driven by many-body interactions
Technical University of Munich（慕尼黑工业大学）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；National Institute for Materials Science（物质材料研究机构）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（物质材料研究机构电子光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料研究机构材料纳米架构研究中心）
Monolayer transition metal dichalcogenides (TMDs) possess superior optical properties, including the valley degree of freedom that can be accessed through the excitation light of certain helicity. While WS2 and WSe2 are known for their excellent valley polarization due to the strong spin-orbit coupling, the optical bandgap is limited by the ability to choose from only these two materials. This limitation can be overcome through the monolayer alloy semiconductor, WS2xSe2(1-x), which promises an atomically thin semiconductor with tunable bandgap. In this work, we show that the high-quality BN en…
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…
Twisted bilayer graphene (TwBLG) is one of the simplest van der Waals heterostructures, yet it yields a complex electronic system with intricate interplay between moiré physics and interlayer hybridization effects. We report on electronic transport measurements of high mobility small angle TwBLG devices showing clear evidence for insulating states at the superlattice band edges, with thermal activation gaps several times larger than theoretically predicted. Moreover, Shubnikov-de Haas oscillations and tight binding calculations reveal that the band structure consists of two intersecting Fermi …
Monolayer transition metal dichalcogenides have attracted great attentions for potential applications in valleytronics. However, the valley polarization degree is usually not high because of the intervalley scattering. Here, we demonstrate a largely enhanced valley polarization up to 80\% in monolayer WS$_2$ under non-resonant excitation at 4.2 K using WS$_2$/LaMnO$_3$ thin film heterostructure, which is much higher than that for monolayer WS$_2$ on SiO$_2$/Si substrate with a valley polarization of 15\%. Furthermore, the greatly enhanced valley polarization can be maintained to a high tempera…
Hidden valley dynamics behind vanishing circular polarization in moiré excitons
National Institute for Materials Science（物质材料研究机构）；Graduate School of Chemical Sciences and Engineering, Hokkaido University（北海道大学化学理工学研究科）；University of Tsukuba（筑波大学）
A graphene bilayer in a transverse magnetic field has a set of Landau levels with energies $E=\pm \sqrt{N(N+1)}\hslash ω_{c}^{\ast}$ where $ω_{c}^{\ast}$ is the effective cyclotron frequency and $% N=0,1,2,...$ All Landau levels but N=0 are four times degenerate counting spin and valley degrees of freedom. The Landau level N=0 has an extra degeneracy due to the fact that orbitals $n=0$ and $n=1$ both have zero kinetic energies. At integer filling factors, Coulomb interactions produce a set of broken-symmetry states with partial or full alignement in space of the valley and orbital pseudospins.…
Van der Waals heterostructures offer attractive opportunities to design quantum materials. For instance, transition metal dichalcogenides (TMDs) possess three quantum degrees of freedom: spin, valley index, and layer index. Further, twisted TMD heterobilayers can form moiré patterns that modulate the electronic band structure according to atomic registry, leading to spatial confinement of interlayer exciton (IXs). Here we report the observation of spin-layer locking of IXs trapped in moiré potentials formed in a heterostructure of bilayer 2H-MoSe$_2$ and monolayer WSe$_2$. The phenomenon of lo…
Van der Waals heterostructures made of graphene and transition metal dichalcogenides (TMD) are an emerging platform for opto-electronic, -spintronic and -valleytronic devices that could benefit from (i) strong light-matter interactions and spin-valley locking in TMDs and (ii) exceptional electron and spin transport in graphene. The operation of such devices requires significant valley polarization and valley coherence, ideally up to room temperature. Here, using a comprehensive Mueller polarimetry analysis, we report \textit{artifact-free} room temperature degrees of valley polarization up to …
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…
Twisted layers of atomically thin two-dimensional materials realize a broad range of novel quantum materials with engineered optical and transport phenomena arising from spin and valley degrees of freedom and strong electron correlations in hybridized interlayer bands. Here, we report experimental and theoretical studies of WSe$_2$ homobilayers obtained in two stable configurations of 2H ($60^\circ$ twist) and 3R ($0^\circ$ twist) stackings by controlled chemical vapor synthesis of high-quality large-area crystals. Using optical absorption and photoluminescence spectroscopy at cryogenic temper…
Moiré superlattices in atomically thin van-der-Waals heterostructures hold great promise for an extended control of electronic and valleytronic lifetimes, the confinement of excitons in artificial moiré lattices, and the formation of novel exotic quantum phases. Such moiré-induced emergent phenomena are particularly strong for interlayer excitons, where the hole and the electron are localized in different layers of the heterostructure. In order to exploit the full potential of correlated moiré and exciton physics, a thorough understanding of the ultrafast interlayer exciton formation process a…
Charge carriers in two-dimensional transition metal dichalcogenides (TMDs), such as WSe$_2$, have their spin and valley-pseudospin locked into an optically-addressable index that is proposed as a basis for future information processing. The manipulation of this spin-valley index requires tuning its energy, typically through external magnetic field (B), which is cumbersome. Thus, other efficient routes like all-optical control of spin-valley index are desirable. Here, we show that many-body interactions amongst interlayer excitons in WSe$_2$/MoSe$_2$ heterobilayer induce a steady-state valley Z…
The valley of transition metal dichalcogenides provides an additional platform to manipulate spin due to its unique selection rule. Normally, intralayer optical transitions in magnetic field show a Zeeman splitting with g factor of about $-4$. Here we report remarkable valley Zeeman effect exhibited by splitting of excitonic emission in a bilayer WS$_{2}$, with a value of g factor as large as $-16.5$. The observed large g factor results from the interlayer recombination, as the conduction band and valence band are modified in opposite directions by magnetic field in different layers. The inter…
Transition metal dichalcogenides (TMDs) have valley degree of freedom, which features optical selection rule and spin-valley locking, making them promising for valleytronics devices and quantum computation. For either application, a long valley polarization lifetime is crucial. Previous results showed that it is around picosecond in monolayer excitons, nanosecond for electrons, holes or local excitons and tens of nanosecond for interlayer excitons. Here we show that dark excitons in 2D heterostructures provide a microsecond valley polarization memory thanks to the magnetic field induced suppre…
