We report the first experimental observation of strong coupling effect in one-dimensional moiré crystals. We study one-dimensional double-wall carbon nanotubes (DWCNTs) in which van der Waals-coupled two single nanotubes form one-dimensional moiré superlattice. We experimentally combine Rayleigh scattering spectroscopy and electron beam diffraction on the same individual DWCNTs to probe the optical transitions of structure-identified DWCNTs in the visible spectral range. Among more than 30 structure-identified DWCNTs examined, we experimentally observed and identified a drastic change of optical transition spectrum in DWCNT with chirality (12,11)@(17,16). The origin of the marked change is attributed to the strong intertube coupling effect in a moiré superlattice formed by two nearly-armchair nanotubes. Our numerical simulation is consistent to these experimental findings.
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）
Interference effects in finite sections of one-dimensional moiré crystals are investigated using a Landauer-Büttiker formalism within the tight-binding approximation. We explain interlayer transport in double-wall carbon nanotubes and design a predictive model. Wave function interference is visible at the mesoscale: in the strong coupling regime, as a periodic modulation of quantum conductance and emergent localized states; in the localized-insulating regime, as a suppression of interlayer transport, and oscillations of the density of states. These results could be exploited to design quantum …
In heterostructures consisting of atomically thin crystals layered on top of one another, lattice mismatch or rotation between the layers results in long-wavelength moiré superlattices. These moiré patterns can drive significant band structure reconstruction of the composite material, leading to a wide range of emergent phenomena including superconductivity, magnetism, fractional Chern insulating states, and moiré excitons. Here, we investigate monolayer graphene encapsulated between two crystals of boron nitride (BN), where the rotational alignment between all three components can be varied. …
Layer-Hybridized Wigner Crystals in MoSe2/WS2 Moiré Superlattice
Carnegie Mellon University（卡内基梅隆大学）；Arizona State University（亚利桑那州立大学）；National Institute for Materials Science（国立材料研究所）；The University of Texas at Dallas（德克萨斯大学达拉斯分校）；University of California at Riverside（加州大学河滨分校）
Moiré superlattices are emerging as a new route for engineering strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states in magic-angle twisted bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices. Transition metal dichalcogenide (TMDC) moiré heterostructures provide another exciting model system to explore correlated quantum phenomena, with the addition of strong light-matter interactions and large spin-orbital coupling. Here we report the optical detection …
Formation of moiré superlattices is common in Van der Waals heterostructures as a result of the mismatch between lattice constants and misalignment of crystallographic directions of the constituent two-dimensional crystals. We discuss theoretically electron transport in a Van der Waals tunnelling transistor in which one of the electrodes is made of two crystals forming a moiré superlattice at their interface. By investigating structures containing either the aligned graphene/hexagonal boron nitride heterostructure or twisted bilayer graphene, we show that negative differential resistance is po…
Graphene is an atomically thin plasmonic medium that supports highly confined plasmon polaritons, or nano-light, with very low loss. Electronic properties of graphene can be drastically altered when it is laid upon another graphene layer, resulting in a moiré superlattice. The relative twist angle between the two layers is a key tuning parameter of the interlayer coupling in thus obtained twisted bilayer graphene (TBG). We studied propagation of plasmon polaritons in TBG by infrared nano-imaging. We discovered that the atomic reconstruction occurring at small twist angles transforms the TBG in…
We explore the skyrmion formation and control possibilities in 2D magnets from the ubiquitous moiré pattern in vdW heterostructures. Using the example of a ferromagnetic monolayer on an antiferromagnetic substrate, we demonstrate a new origin of skyrmions in the 2D magnets, from the lateral modulation of interlayer magnetic coupling by the locally different atomic registries in moiré. The moiré skyrmions are doubly degenerate with opposite topological charge, and trapped at an ordered array of sites with the moiré periodicity that can be dramatically tuned by strain and interlayer translation.…
Ab-Initio Theory of Moiré Superlattice Bands in Layered Two-Dimensional Materials
当原子级薄的二维（2D）材料被分层时，它们通常形成不相称的非晶体结构，当通过扫描探针检查时，这些结构表现出长周期莫尔图案。在本文中，我们提出了一种方法，它使用从{ \it ab initio}计算获得的信息进行短周期晶体结构，以获得有效的哈密顿量，能够有效地描述莫尔{\' e}图案超晶格的电子性质的影响。我们将我们的方法应用于石墨烯上的石墨烯（G/G）和六方氮化硼上的石墨烯（G/BN）的情况，推导出具有莫尔图案的周期性的显式有效哈密顿量，并且可以用于计算任意扭曲角和晶格常数的感兴趣的电子性质。
In stacks of two-dimensional crystals, mismatch of their lattice constants and misalignment of crystallographic axes lead to formation of moiré patterns. We show that moiré superlattice effects persist in twisted bilayer graphene (tBLG) with large twists and short moiré periods. Using angle-resolved photoemission, we observe dramatic changes in valence band topology across large regions of the Brillouin zone, including the vicinity of the saddle point at $M$ and across 3 eV from the Dirac points. In this energy range, we resolve several moiré minibands and detect signatures of secondary Dirac …
In moiré crystals formed by stacking van der Waals (vdW) materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS$_2$ twisted bilayers, adding a new perspective to moiré physics. Over a range of small twist angles, the phonon spectra evolve rapidly due to ultra-strong coupling between different phonon modes and atomic reconstructions of the moiré pattern. We develop a new low-energy continuum model for phonons that overcomes the outstanding challe…
In twisted bilayers of semiconducting transition metal dichalcogenides (TMDs), a combination of structural rippling and electronic coupling gives rise to periodic moiré potentials that can confine charged and neutral excitations. Here, we report experimental measurements of the structure and spectroscopic properties of twisted bilayers of WSe2 and MoSe2 in the H-stacking configuration using scanning tunneling microscopy (STM). Our experiments reveal that the moiré potential in these bilayers at small angles is unexpectedly large, reaching values of above 300 meV for the valence band and 150 me…
We investigate the physics of photonic band structures of the moiré patterns that emerged when overlapping two uni-dimensional (1D) photonic crystal slabs with mismatched periods. The band structure of our system is a result of the interplay between intra-layer and inter-layer coupling mechanisms, which can be fine-tuned via the distance separating the two layers. We derive an effective Hamiltonian that captures the essential physics of the system and reproduces all numerical simulations of electromagnetic solutions with high accuracy. Most interestingly, \textit{magic distances} corresponding…
Many-body interactions between carriers lie at the heart of correlated physics. The ability to tune such interactions would open the possibility to access and control complex electronic phase diagrams on demand. Recently, moiré superlattices formed by two-dimensional materials have emerged as a promising platform for quantum engineering such phenomena. The power of the moiré system lies in the high tunability of its physical parameters by tweaking layer twist angle, electrical field, moiré carrier filling, and interlayer coupling. Here, we report that optical excitation can drastically tune th…
We theoretically study a generalized Hubbard model on moiré superlattices of twisted bilayers, and find very rich filling-factor-dependent quantum phase diagrams tuned by interaction strength and twist angle. Strong long-range Coulomb interaction in the moiré-Hubbard model induces Wigner crystals at a series of fractional filling factors. The effective lattice of the Wigner crystal is controlled by the filling factor, and can be triangle, rectangle, honeycomb, kagome, etc, providing a single platform to realize many different spin models on various lattices by simply tuning carrier density. In…
The Wigner crystal state, first predicted by Eugene Wigner in 1934, has fascinated condensed matter physicists for nearly 90 years2-14. Studies of two-dimensional (2D) electron gases first revealed signatures of the Wigner crystal in electrical transport measurements at high magnetic fields2-4. More recently optical spectroscopy has provided evidence of generalized Wigner crystal states in transition metal dichalcogenide (TMDC) moiré superlattices. Direct observation of the 2D Wigner crystal lattice in real space, however, has remained an outstanding challenge. Scanning tunneling microscopy (S…
Ultrathin iron oxide films epitaxially grown on the (111)- and (0001)-oriented metal single crystal supports exhibit unique electronic, catalytic and magnetic properties not observed for the corresponding bulk oxides. These properties originate mainly from the presence of Moiré superstructures which, in turn, disqualify ultrathin films as model systems imitating bulk materials. We present a route for the preparation of a close-packed Moiré-free ultrathin iron oxide film, namely FeO(111) on Ag(111). Experimental scanning tunneling microscopy (STM), low energy electron diffraction (LEED) and x-r…
Nanyang Technological University（南洋理工大学）；Sun Yat-Sen University (Zhuhai Campus)（中山大学（珠海校区））；Nanjing University of Aeronautics and Astronautics（南京航空航天大学）；École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；National Institute for Materials Science（物质材料研究机构）；University of Science and Technology of China（中国科学技术大学）；Sun Yat-Sen University (Guangzhou Campus)（中山大学（广州校区））
Recent experiments on the twisted transition metal dichalcogenide (TMD) material, $\rm WSe_2/WS_2$, have observed insulating states at fractional occupancy of the moiré bands. Such states were conceived as generalized Wigner crystals (GWCs). In this article, we investigate the problem of Wigner crystallization in the presence of an underlying (moiré) lattice. Based on the best estimates of the system parameters, we find a variety of homobilayer and heterobilayer TMDs to be excellent candidates for realizing GWCs. In particular, our analysis based on $r_{s}$ indicates that $\rm MoSe_{2}$ (among…
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…
Flexible long period moir\' e superlattices form in two-dimensional van der Waals crystals containing layers that differ slightly in lattice constant or orientation. In this Letter we show theoretically that isolated flat moir\' e bands described by generalized triangular lattice Hubbard models are present in twisted transition metal dichalcogenide heterobilayers. The hopping and interaction strength parameters of the Hubbard model can be tuned by varying the twist angle and the three-dimensional dielectric environment. When the flat moiré bands are partially filled, candidate many-body ground…
Twisted van der Waals heterostructures and the corresponding superlattices, moire superlattices, are remarkable new material platforms, in which electron interactions and excited-state properties can be engineered. Particularly, the band offsets between adjacent layers can separate excited electrons and holes, forming interlayer excitons that exhibit unique optical properties. In this work, we employ the first-principles GW-Bethe-Salpeter Equation (BSE) method to calculate quasiparticle band gaps, interlayer excitons, and their modulated excited-state properties in twisted MoSe2/WSe2 bilayers …
Imaging moiré flat bands and Wigner molecular crystals in twisted bilayer MoTe2
Tsung-Dao Lee Institute, Shanghai Jiao Tong University（上海交通大学李政道研究所）；Key Laboratory of Artificial Structures and Quantum Control (Ministry of Education), School of Physics and Astronomy, Shanghai Jiao Tong University（上海交通大学物理与天文学院人工结构与量子控制教育部重点实验室）；Department of Physics and Astronomy, University of Tennessee（田纳西大学物理与天文系）；Department of Physics, Tsinghua University（清华大学物理系）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（日本国立材料研究所电子光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（日本国立材料研究所材料纳米结构研究中心）；Hefei National Laboratory（合肥国家实验室）；Min H. Kao Department of Electrical Engineering and Computer Science, University of Tennessee（田纳西大学明海华电气与计算机工程系）
Unlike conventional two-dimensional (2D) semiconductor superlattices, moiré patterns in 2D materials are flexible and their electronic, magnetic, optical, and mechanical properties depend on their topography. Within a continuous+atomistic theory treating 2D materials as crystalline elastic membranes, we abandon the flat-membrane scenario usually assumed for these materials and address out-of-plane deformations. We confront our predictions to experimental analyses on model systems, epitaxial graphene, and MoS$_2$ on metals and reveal that compression/expansion and bending energies stored in the…
The relative orientation (twist) of successive layers of stacked two-dimensional (2D) materials creates variations in the interlayer atomic registry. The variations often form a super lattice, called a moiré pattern, which can alter electronic properties. In this work we introduce a classification of the single-particle electronic structures that can occur in twisted stacks of 2D layers by characterizing them as "moiré molecules" or "moiré crystals". The molecules generate localized electronic states and moiré flat bands, while the crystals are sometimes unconventional and produce electronic b…
When two-dimensional atomic crystals are brought into close proximity to form a van der Waals heterostructure, neighbouring crystals can start influencing each others electronic properties. Of particular interest is the situation when the periodicity of the two crystals closely match and a moiré pattern forms, which results in specific electron scattering, reconstruction of electronic and excitonic spectra, crystal reconstruction, and many other effects. Thus, formation of moiré patterns is a viable tool of controlling the electronic properties of 2D materials. At the same time, the difference…
Large scale two-dimensional (2D) moiré superlattices are driving a revolution in designer quantum materials. The electronic interactions in these superlattices, strongly dependent on the periodicity and symmetry of the moiré pattern, critically determine the emergent properties and phase diagrams. To date, the relative twist angle between two layers has been the primary tuning parameter for a given choice of constituent crystals. Here, we establish strain as a powerful mechanism to in-situ modify the moiré periodicity and symmetry. We develop an analytically exact mathematical description for …
We present a low-energy model describing the reconstruction of the electronic spectrum in twisted bilayers of honeycomb crystals with broken sublattice symmetry. The resulting moiré patterns are classified into two families with different symmetry. In both cases, flat bands appear at relatively large angles, without any magic angle condition. Transitions between them give rise to sharp resonances in the optical absorption spectrum at frequencies well below the gap of the monolayer. Owing to their chiral symmetry, twisted bilayers display circular dichroism, i.e., different absorption of left a…
University of Southern California（南加州大学）；Tamkang University（淡江大学）；The University of British Columbia（不列颠哥伦比亚大学）；The University of Texas at Austin（德克萨斯大学奥斯汀分校）；University of Washington（华盛顿大学）；University of California at Berkeley（加利福尼亚大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）
Moiré materials provide a highly tunable environment for the realization of band structures with engineered physical properties. Specifically, moiré structures with Fermi surface flat bands - a synthetic environment for the realization of correlated phases - have moiré unit cells containing thousands of atoms and tantalizingly complex bands structures. In this paper we show that statistical principles go a long way in explaining universal physical properties of these systems. Our approach builds on three conceptual elements: the presence of quantum chaos caused by the effective irregularity of…
Monolayer islands of molybdenum disulfide (MoS$_2$) on Au(111) form a characteristic moiré structure, leading to locally different stacking sequences at the S-Mo-S-Au interface. Using low-temperature scanning tunneling microscopy (STM) and atomic force microscopy (AFM), we find that the moiré islands exhibit a unique orientation with respect to the Au crystal structure. This indicates a clear preference of MoS$_2$ growth in a regular stacking fashion. We further probe the influence of the local atomic structure on the electronic properties. Differential conductance spectra show pronounced feat…
Stripe phases, in which the rotational symmetry of charge density is spontaneously broken, occur in many strongly correlated systems with competing interactions. One representative example is the copper-oxide superconductors, where stripe order is thought to be relevant to the mechanism of high-temperature superconductivity. Identifying and studying the stripe phases in conventional strongly correlated systems are, however, challenging due to the complexity and limited tunability of these materials. Here we uncover stripe phases in WSe2/WS2 moiré superlattices with continuously gate-tunable ch…
