We develop a general theory for how an exciton in an atomically thin transition metal dichacogenide (TMD) monolayer couples to spin and charge correlations in an adjacent moire lattice created by a TMD bi-layer. Virtual tunneling of charge carriers, assumed for concreteness to be holes, between the moire lattice and the monolayer combined with the presence of bound hole-exciton states, i.e. trions, give rise to an effective interaction between the moire holes and the exciton. In addition to the Umklapp scattering, we show that this interaction is spin-dependent and therefore couples the exciton to the spin correlations of the moire holes, which may be in- as well as out-of-plane. We then use our theory to examine two specific examples where the moire holes form in-plane ferromagnetic or anti-ferromagnetic order. In both cases, the exciton creates spin waves in the moire lattice, which we analyse by using a self-consistent Born approximation that includes such processes to infinite order. We show that the competition between magnetic order and exciton motion leads to the formation of a well-defined quasiparticle consisting of the exciton surrounded by a cloud of magnetic frustration in the moire lattice sites below. For the anti-ferromagnet, we furthermore demonstrate the presence of the elusive geometric string excitations and discuss how they can be observed via their smoking gun energy dependence on the spin-spin coupling, which can be tuned by varying the twist angle of the moire bi-layer. All these phenomena have clear signatures in the exciton spectrum, and as such our results illustrate that excitons are promising probes providing optical access to the spin correlations of new quantum phases predicted to exist in TMD materials.
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…
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 …
We investigate the optical properties of interlayer excitons in heterobilayer transition metal dichalcogenides where moiré pattern is introduced by heterostrain, in comparison with that introduced by twisting (and/or lattice mismatch). Besides being a cause of the moiré texture, strain also effectively introduces a constant gauge potential on either electron or hole, which shifts the dispersion of kinetic energy with respect to the excitonic crystal momenta in the moiré superlattices.This leads to distinct exciton mini-band dispersions and light coupling properties from the twisting induced mo…
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…
Observation of an exciton crystal in a moiré excitonic insulator
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；National Institute for Materials Science（物质材料研究机构）；Kavli Energy NanoScience Institute（卡弗里纳米科学能源研究所）
Moiré patterns are common in Van der Waals heterostructures and can be used to apply periodic potentials to elementary excitations. We show that the optical absorption spectrum of transition metal dichalcogenide bilayers is profoundly altered by long period moiré patterns that introduce twist-angle dependent satellite excitonic peaks. Topological exciton bands with non-zero Chern numbers that support chiral excitonic edge states can be engineered by combining three ingredients: i) the valley Berry phase induced by electron-hole exchange interactions, ii) the moiré potential, and iii) the valle…
Moiré exciton features tunable Dirac dispersion and spatially dependent optical selection rules. With the long lifetime due to its interlayer nature, it is promising to realize a Bose-Einstein condensation of moiré excitons. Here we study the properties of moiré exciton condensate within the mean-field theory, with special focus on exciton-exciton interaction effect on the nonlinear Bloch band and Bloch waves of exciton condensate in moiré potential. We find the nonlinear dispersion of the moiré exciton condensate exhibits complex loop structure induced by exciton-exciton interaction. A nonlin…
Cascade transition between energy levels has important applications, such as in quantum information protocols and quantum cascade lasers. In two-dimensional heterostructure, the moiré superlattice potential can result in multiple interlayer exciton (IX) energy levels. We demonstrate the cascade transitions between such moiré IXs by performing time- and energy-resolved photoluminescence measurements. We show that the lower-energy moiré IX can be excited to higher-energy ones, facilitating IX population inversion.
Moiré heterostructures are rapidly emerging as a tunable platform to study correlated electronic phenomena. Discovery of exotic quantum phases in moiré systems requires novel probes of charge and spin order. Unlike detection schemes which average over several moiré cells, local sensors can provide richer information with greater sensitivity. We study a WSe$_2$/MoSe$_2$/WSe$_2$ heterotrilayer which hosts excitons and electrons in distinct moiré lattices, and show that localized dipolar excitons are sensitive proximity charge sensors, uncovering numerous correlated electronic states at fractiona…
Moiré superlattices formed in van der Waals bilayers have enabled the creation and manipulation of new quantum states, as is exemplified by the discovery of superconducting and correlated insulating states in twisted bilayer graphene near the magic angle. Twisted bilayer semiconductors may lead to tunable exciton lattices and topological states, yet signatures of moiré excitons have been reported only in closely angularly-aligned bilayers. Here we report tuning of moiré lattice in WS$_{2}$ /MoSe$_{2}$ bilayers over a wide range of twist angles, leading to the continuous tuning of moiré lattice…
Stacking transition metal dichalcogenides (TMDs) to form moiré superlattices has provided exciting opportunities to explore many-body correlation phenomena of the moiré trapped carriers. TMDs bilayers, on the other hand, host long-lived interlayer exciton (IX), an elementary excitation of long spin-valley lifetime that can be optically or electrically injected. Here we find that, through the Coulomb exchange between mobile IXs and carriers, the IX bath can mediate both Heisenberg and Dzyaloshinskii-Moriya type spin interactions between moiré trapped carriers, controllable by exciton density an…
Moiré lattices formed from semiconductor bilayers host tightly localised excitons that can simultaneously couple strongly to light and possess large electric dipole moments. This facilitates the realization of new forms of polaritons that are very strongly interacting and that have been predicted to lead to strong optical nonlinearities controlled by multi-photon resonances. Here, we investigate the role of the non-local component of the exciton-exciton (dipolar) interactions on the optical response of these strongly-interacting moiré exciton-polaritons under conditions of strong optical drivi…
We present a detailed investigation of excitonic absorption in $Zn_{0.69}Cd_{0.31}Se/ZnSe$ quantum wells under the application of a perpendicular magnetic field. The large energy separation between heavy- and light-hole excitons allows us to clearly resolve and identify magneto-excitonic absorption resonant with the continuum edge of the 1S heavy-hole exciton. Experimental values of the exciton binding energy are compared with results of a theoretical model that includes the exciton-phonon interaction. The remarkable agreemeent found unambiguously indicates the predominant polaronic character …
Exciton-polaron Umklapp scattering in Wigner crystals
University of California, Riverside（加州大学河滨分校）；Nanjing University（南京大学）；Stanford University（斯坦福大学）；SLAC National Accelerator Laboratory（SLAC国家加速器实验室）；National Institute for Materials Science（国立材料研究所）；Academia Sinica（中央研究院）；National Cheng Kung University（国立成功大学）
Photon antibunching, a hallmark of quantum light, has been observed in the correlations of light from isolated atomic and atomic-like solid-state systems. Two-dimensional semiconductor heterostructures offer a unique method to create a quantum light source: a small lattice mismatch or relative twist in a heterobilayer can create moiré trapping potentials for excitons which are predicted to create arrays of quantum emitters. While signatures of moiré trapped excitons have been observed, their quantum nature has yet to be confirmed. Here we report photon antibunching from single moiré trapped in…
In previous work we have argued that the optical properties of moderately doped two-dimensional semiconductors can be described in terms of excitons dressed by their interactions with a degenerate Fermi sea of additional charge carriers. These interactions split the bare exciton into attractive and repulsive exciton-polaron branches. The collective excitations of the coupled system are many-body generalizations of the bound trion and unbound states of a single electron interacting with an exciton. In this article we consider exciton-polarons in the presence of an external magnetic field that q…
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…
In twisted homobilayer transition metal dichalcogenides, intra- and inter-layer valley excitons hybridize with the layer configurations spatially varying in the moiré. The ground state valley excitons are trapped at two high-symmetry points with opposite electric dipoles in a moiré supercell, forming a honeycomb superlattice of nearest-neighbor dipolar attraction. We find that the spatial texture of layer configuration results in a luminescence anomaly of the moiré trapped excitons, where a tiny displacement by interactions dramatically increases the brightness and changes polarization from ci…
Recently, it has been demonstrated that the absorption of moderately doped two-dimensional semiconductors can be described in terms of exciton-polarons. In this scenario, attractive and repulsive polaron branches are formed due to interactions between a photo-excited exciton and a Fermi sea of excess charge carriers. These interactions have previously been treated in a phenomenological manner. Here, we present a microscopic derivation of the electron-exciton interactions which utilizes a mixture of variational and perturbative approaches. We find that the interactions feature classical charge-…
Transition-metal dichalcogenide heterostructures exhibit moiré patterns that spatially modulate the electronic structure across the material's plane. For certain material pairs, this modulation acts as a potential landscape with deep, trigonally symmetric wells capable of localizing interlayer excitons, forming periodic arrays of quantum emitters. Here, we study these moiré localized exciton states and their optical properties. By numerically solving the two-body problem for an interacting electron-hole pair confined by a trigonal potential, we compute the localized exciton spectra for differe…
Moiré superlattices in van der Waals heterostructures have emerged as a powerful tool for engineering novel quantum phenomena. Here we report the observation of a correlated interlayer exciton insulator in a double-layer heterostructure composed of a WSe2 monolayer and a WS2/WSe2 moiré bilayer that are separated by an ultrathin hexagonal boron nitride (hBN). The moiré WS2/WSe2 bilayer features a Mott insulator state at hole density p/p0 = 1, where p0 corresponds to one hole per moiré lattice site. When electrons are added to the Mott insulator in the WS2/WSe2 moiré bilayer and an equal number …
Moiré superlattices in twisted van der Waals materials constitute a promising platform for engineering electronic and optical properties. However, a major obstacle to fully understanding these systems and harnessing their potential is the limited ability to correlate the local moiré structure with optical properties. By using a recently developed scanning electron microscopy technique to image twisted WSe$_2$/WSe$_2$ bilayers, we directly correlate increasing moiré periodicity with the emergence of two distinct exciton species. These can be tuned individually through electrostatic gating, and …
The propagation of excitons in TMD monolayers has been intensively studied revealing interesting many-particle effects, such as halo formation and non-classical diffusion. Initial studies have investigated how exciton transport changes in twisted TMD bilayers, including Coulomb repulsion and Hubbard-like exciton hopping. In this work, we investigate the twist-angle-dependent transition of the hopping regime to the dispersive regime of effectively free excitons. Based on a microscopic approach for excitons in the presence of a moiré potential, we show that the hopping regime occurs up to an ang…
Recent advances in the field of vertically stacked 2D materials have revealed a rich exciton landscape. In particular, it has been demonstrated that out-of-plane electrical fields can be used to tune the spectral position of spatially separated interlayer excitons. Other studies have shown that there is a strong hybridization of exciton states, resulting from the mixing of electronic states in both layers. However, the connection between the twist-angle dependent hybridization and field-induced energy shifts has remained in the dark. Here, we investigate on a microscopic footing the interplay …
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…
The large surface-to-volume ratio in atomically thin 2D materials allows to efficiently tune their properties through modifications of their environment. Artificial stacking of two monolayers into a bilayer leads to an overlap of layer-localized wave functions giving rise to a twist angle-dependent hybridization of excitonic states. In this joint theory-experiment study, we demonstrate the impact of interlayer hybridization on bright and momentum-dark excitons in twisted WSe$_2$ bilayers. In particular, we show that the strong hybridization of electrons at the $Λ$ point leads to a drastic reds…
Two-dimensional moiré materials provide a highly tunable platform to investigate strongly correlated electronic states. Such emergent many-body phenomena can be optically probed in moiré systems created by stacking two layers of transition metal dichalcogenide semiconductors: optically injected excitons can interact with itinerant carriers occupying narrow moiré bands to form exciton-polarons sensitive to strong correlations. Here, we investigate the behaviour of excitons dressed by a Fermi sea localised by the moiré superlattice of a molybdenum diselenide (MoSe$_2$) / tungsten diselenide (WSe…
Moiré patterns with angular mismatch in van der Waals heterostructures composed of atomically thin semiconducting materials are a fascinating platform to engineer the optically generated excitonic properties towards novel quantum phenomena. The moiré pattern as a periodic trap potential can give rise to spatially ordered zero-dimensional (0D) exciton ensembles, which offers the possibility for dense coherent quantum emitters and quantum simulation of many-body physics. The intriguing moiré exciton properties are affected by their dynamics and exciton-phonon interaction. However, the moiré exci…
Spatially periodic structures with a long range period, referred to as moiré pattern, can be obtained in van der Waals bilayers in the presence of a small stacking angle or of lattice mismatch between the monolayers. Theoretical predictions suggest that the resulting spatially periodic variation of the band structure modifies the optical properties of both intra and interlayer excitons of transition metal dichalcogenides heterostructures. Here, we report on the impact of the moiré pattern formed in a MoSe$_2$/MoS$_2$ heterobilayer encapsulated in hexagonal boron nitride. The periodic in-plane …
(Sub)nanoscale Visualization of Reconstruction-Driven Moiré Exciton Localization and Delocalization
Molecular Foundry, Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室分子发现中心）；School for Engineering of Matter, Transport and Energy, Arizona State University（亚利桑那州立大学物质、运输与能源工程学院）；Department of Physics, University of Texas at Austin（德克萨斯大学奥斯汀分校物理系）；National Institute for Materials Science（日本国立材料研究所）；Center for Nanophase Materials Sciences, Oak Ridge National Laboratory（橡树岭国家实验室纳米材料科学中心）；Oden Institute for Computational Engineering and Sciences, The University of Texas at Austin（德克萨斯大学奥斯汀分校奥登计算工程与科学学院）；McKetta Department of Chemical Engineering, The University of Texas at Austin（德克萨斯大学奥斯汀分校麦凯塔化学工程系）；Kavli Energy NanoScience Institute, University of California Berkeley（加州大学伯克利分校卡弗里能源纳米科学研究所）；Jawaharlal Nehru Centre for Advanced Scientific Research（贾瓦哈拉尔·尼赫鲁高级科学研究中心）
Robust valley-polarized excitonic Mott states and doublons enabled by stacking-controlled moiré geometry
National Taiwan University（国立台湾大学）；University of Washington（华盛顿大学）；National Institute for Materials Science（国家材料研究所）；Arizona State University（亚利桑那州立大学）
It has been shown, that a magnetopolaron discrete energy spectrum is realized in the optical experiments where exciting light is directed perpendicularly to a quantum well (QW) plane. The phonon dispersion as well as Coulomb attraction can only shift the magnetopolaron discrete energy levels and broad some of them.
Unveiling the Spin-Valley Structure of Dipolar Exciton Ladders in R-stacked WSe$_2$/WS$_2$ Moiré Heterobilayers
Institute of Photonics and Quantum Sciences, SUPA, Heriot-Watt University（赫瑞-瓦特大学光子与量子科学研究所）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料纳米结构研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（电子与光学材料研究中心）
研究 R 堆叠 WSe₂/WS₂ 莫尔异质双层中偶极激子阶梯的自旋-谷结构，用螺旋度分辨磁光致发光确定其微观起源，明确不同电荷填充时各激子态情况，建立超越简单占据数物理的自旋-谷分辨图像。
Hybrid Perovskites have shown a great potential for applications in photovoltaics and light-emitting devices with high efficiency. Interaction between defect-induced trapped excitons and phonons plays an important role in understanding the emerging phenomena for such an excellent figure-of-merit. Here we demonstrate hot polarons with narrow linewidth in $\mathrm{CH_{3}NH_{3}PbBr_{3}}$ nanowires, which originate from the interaction between trapped excitons and octahedra-twist phonons. The observation of hot polarons in photoluminescence without gain methods indicates the large interaction stre…
Moire superlattices in van der Waals (vdW) heterostructures could trap strongly bonded and long lived interlayer excitons. Assumed to be localized, these moire excitons could form ordered quantum dot arrays, paving the way for novel optoelectronic and quantum information applications. Here we perform first principles simulations to shed light on moire excitons in twisted MoS2/WS2 heterostructures. We provide the direct evidence of localized interlayer moire excitons in vdW heterostructures. The moire potentials are mapped out based on spatial modulations of energy gaps. Nearly flat valence ban…
