We demonstrate that the concept of moiré flat bands can be generalized to achieve electronic band engineering in all three spatial dimensions. For many two dimensional van der Waals materials, twisting two adjacent layers with respect to each other leads to flat electronic bands in the two corresponding spatial directions -- a notion sometimes referred to as twistronics as it enables a wealth of physical phenomena. Within this two dimensional plane, large moiré patterns of nanometer size form. The basic concept we propose here is to stack multiple twisted layers on top of each other in a predefined pattern. If the pattern is chosen such that with respect to the stacking direction of layers, the large spatial moiré features are spatially shifted from one twisted layer to the next, the system exhibits twist angle controlled flat bands in all of the three spatial directions. With this, our proposal extends the use of twistronic to three dimensions. We exemplify the general concept by considering graphitic systems, boron nitride and WSe$_2$ as candidate materials, but the approach is applicable to any two-dimensional van der Waals material. For hexagonal boron nitride we develope an ab initio fitted tight binding model that captures the corresponding three dimensional low-energy electronic structure. We outline that interesting three dimensional correlated phases of matter can be induced and controlled following this route, including quantum magnets and unconventional superconducting states.
Moire superlattices in twisted bilayer graphene (TBG) and its derived structures can host exotic correlated quantum phenomena because the narrow moire flat minibands in those systems effectively enhance the electron-electron interaction. Correlated phenomena are also observed in 2H-transitional metal dichalcogenides moire superlattices. However, the number of moire systems that have been explored in experiments are still very limited. Here we theoretically investigate a series of two-dimensional (2D) twisted bilayer hexagonal materials (TBHMs) beyond TBG at fixed angles of 7.34 and 67.34 degre…
Moiré heterostructures hold the promise to provide platforms to tailor strongly correlated and topological states of matter. Here, we theoretically propose the emergence of an effective, rectangular moiré lattice in twisted bilayers of SnS with nonsymmorphic symmetry. Based on first-principles calculations, we demonstrate that strong intrinsic spin-orbit interactions render this tunable platform a moiré semimetal that hosts 2D hourglass fermions protected by time-reversal symmetry $\mathcal{T}$ and the nonsymmorphic screw rotation symmetry $\widetilde{\mathcal{C}}_{2y}$. We show that topologic…
Moiré engineering has recently emerged as a capable approach to control quantum phenomena in condensed matter systems. In van der Waals heterostructures, moiré patterns can be formed by lattice misorientation between adjacent atomic layers, creating long range electronic order. To date, moiré engineering has been executed solely in stacked van der Waals multilayers. Herein, we describe our discovery of electronic moiré patterns in films of a prototypical magnetoresistive oxide La0.67Sr0.33MnO3 (LSMO) epitaxially grown on LaAlO3 (LAO) substrates. Using scanning probe nano-imaging, we observe mi…
Recently, artificial moire superlattices of classical waves have aroused tremendous interest, inspired by the newly emergent twistronics that focuses on the peculiar electronic properties induced by flat bands. However, so far, the moire flat bands have not been observed directly. Here, we report the first experimental observation of ultraflat bands in moire sonic crystals with frequency-momentum spectra, together with a real-space visualization of the hallmark localized states. Strikingly different from the established magic angle mechanism for twisted bilayer graphene, the flat bands are for…
Moiré superlattices in transition metal dichalcogenide (TMD) heterostructures can host novel correlated quantum phenomena due to the interplay of narrow moiré flat bands and strong, long-range Coulomb interactions1-5. However, microscopic knowledge of the atomically-reconstructed moiré superlattice and resulting flat bands is still lacking, which is critical for fundamental understanding and control of the correlated moiré phenomena. Here we quantitatively study the moiré flat bands in three-dimensional (3D) reconstructed WSe2/WS2 moiré superlattices by comparing scanning tunneling spectroscop…
We predict that twisted bilayers of 1T-ZrS$_2$ realize a novel and tunable platform to engineer two-dimensional topological quantum phases dominated by strong spin-orbit interactions. At small twist angles, ZrS$_2$ heterostructures give rise to an emergent and twist-controlled moiré Kagomé lattice, combining geometric frustration and strong spin-orbit coupling to give rise to a moiré quantum spin Hall insulator with highly controllable and nearly-dispersionless bands. We devise a generic pseudo-spin theory for group-IV transition metal dichalcogenides that relies on the two-component character…
Reconfigurable flat bands from cooperative moiré and charge order
University of St Andrews（圣安德鲁斯大学）；Diamond Light Source（钻石光源）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Lund University（隆德大学）
We present a framework that explains the strong connection in 2D materials between mechanics and electronic structure, via dislocation theory. Within this framework, Moiré patterns created by layered 2D materials may be understood as dislocation arrays, and vice versa. The dislocations are of a unique type that we describe as van der Waals dislocations, for which we present a complete geometrical description, connected to both stretch and twist Moiré patterns. A simple computational scheme, which reduces the complexity of the electronic interaction between layers in order to make the problem c…
Tailoring electron transfer dynamics across solid-liquid interfaces is fundamental to the interconversion of electrical and chemical energy. Stacking atomically thin layers with a very small azimuthal misorientation to produce moiré superlattices enables the controlled engineering of electronic band structures and the formation of extremely flat electronic bands. Here, we report a strong twist angle dependence of heterogeneous charge transfer kinetics at twisted bilayer graphene electrodes with the greatest enhancement observed near the 'magic angle' (~1.1 degrees). This effect is driven by th…
We review recent work on low-frequency Floquet engineering and its application to quantum materials driven by light, emphasizing van der Waals systems hosting Moiré superlattices. These non-equilibrium systems combine the twist-angle sensitivity of the band structures with the flexibility of light drives. The frequency, amplitude, and polarization of light can be easily tuned in experimental setups, leading to platforms with on-demand properties. First, we review recent theoretical developments to derive effective Floquet Hamiltonians in different frequency regimes. We apply some of these theo…
We investigate the chirality of phonon modes in twisted bilayer WSe2 and demonstrate distinct chiral behavior of the $K/K^\prime$ valley phonons for twist angles close to $0^{\circ}$ and close to $60^{\circ}$. In particular, multiple chiral non-degenerate $K/K^\prime$ valley phonons are found for twist angles near $60^{\circ}$ whereas no non-degenerate chiral modes are found for twist angles close to $0^\circ$. Moreover, we discover two sets of emergent chiral valley modes that originate from an inversion symmetry breaking at the moiré scale and find similar modes in moiré patterns of strain-e…
We predict that in a twisted homobilayer of transition-metal dichalcogenide MoS$_2$, spin-orbit coupling in the conduction band states from $\pm K$ valleys can give rise to moiré flat bands with nonzero Chern numbers in each valley. The nontrivial band topology originates from a unique combination of angular twist and local mirror symmetry breaking in each individual layer, which results in unusual skyrmionic spin textures in momentum space with skyrmion number $\mathcal{S} = \pm 2$. Our Hartree-Fock analysis further suggests that density-density interactions generically drive the system at $1…
Two-dimensional electronic flat bands and their induced correlated electronic interactions have been discovered, probed, and tuned in interlayer regions of hexagonally shaped van der Waals moire superlattices. Fabrication of anisotropic one-dimensional correlated bands by moire interference of 2D, however, remains a challenge. Here, we report an experimental discovery of 1D electronic flat bands near the Fermi level in an anisotropic rectangular moire superlattice composed of in situ grown, vdW stacked two-atomic-layer thick Bi(110) well-aligned on a SnSe(001) substrate. The epitaxial lattice …
We demonstrate that one-dimensional moiré patterns, analogous to those found in twisted bilayer graphene, can arise in collapsed chiral carbon nanotubes. Resorting to a combination of approaches, namely, molecular dynamics to obtain the relaxed geometries and tight-binding calculations validated against ab initio modeling, we find that magic angle physics occur in collapsed carbon nanotubes. Velocity reduction, flat bands and localization in AA regions with diminishing moiré angle are revealed, showing a magic angle close to 1$^{\rm o}$. From the spatial extension of the AA regions and the wid…
We study the influence of strong spin-orbit interaction on the formation of flat bands in relaxed twisted bilayer WSe$_2$. Flat bands, well separated in energy, emerge at the band edges for twist angles ($θ$) near 0$^{\circ}$ and 60$^{\circ}$. For $θ$ near 0$^{\circ}$, the interlayer hybridization together with a moiré potential determines the electronic structure. The bands near the valence band edge have nontrivial topology, with Chern numbers equal to +1 or $-$1. We propose that the nontrivial topology of the first band can be probed experimentally for twist angles less than a critical angl…
Tsientang Institute for Advanced Study（紫江高等研究院）；Sichuan Normal University（四川师范大学）；Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质结构与动力学研究所）；City University of Hong Kong（香港城市大学）；Songshan Lake Materials Laboratory（松山湖材料实验室）；Center for Computational Quantum Physics (CCQ), The Flatiron Institute（纽约联邦研究所计算量子物理中心）；Donostia International Physics Center (DIPC)（多诺斯蒂亚国际物理中心）；Liaoning University（辽宁大学）
We investigate twisted double bilayer graphene (TDBG), a four-layer system composed of two AB-stacked graphene bilayers rotated with respect to each other by a small angle. Our ab initio band structure calculations reveal a considerable energy gap at the charge point neutrality that we assign to the intrinsic symmetric polarization (ISP). We then introduce the ISP effect into the tight-binding parameterization and perform calculations on TDBG models that include lattice relaxation effects down to very small twist angles. We identify a narrow region around the magic angle $θ^\circ = 1.3^{\circ}…
We explore the moiré magnon bands in twisted bilayer magnets with next-nearest neighboring Dzyaloshinskii-Moriya interactions, assuming that the out-of-plane collinear magnetic order is preserved under weak interlayer coupling. By calculating the magnonic band structures and the topological Chern numbers for four representative cases, we find that (i) the valley moiré bands are extremely flat over a wide range of continuous twist angles; (ii) the topological Chern numbers of the lowest few flat bands vary significantly with the twist angle; and (iii) the lowest few topological flat bands in bi…
Moiré superlattices comprised of stacked two-dimensional materials present a versatile platform for engineering and investigating new emergent quantum states of matter. At present, the vast majority of investigated systems have long moiré wavelengths, but investigating these effects at shorter, incommensurate wavelengths, and at higher energy scales, remains a challenge. Here, we employ angle-resolved photoemission spectroscopy (ARPES) with sub-micron spatial resolution to investigate a series of different moiré superlattices which span a wide range of wavelengths, from a short moiré wavelengt…
Artificially constructed van der Waals heterostructures (vdWHs) provide an ideal platform for realizing emerging quantum phenomena in condensed matter physics. Two methods for building vdWHs have been developed: stacking two-dimensional (2D) materials into a bilayer structure with different lattice constants, or with different orientations. The interlayer coupling stemming from commensurate or incommensurate superlattice pattern plays an important role in vdWHs for modulating the band structures and generating new electronic states. In this article, we review a series of novel quantum states d…
Moiré superlattices that consist of two or more layers of two-dimensional materials stacked together with a small twist angle have emerged as a tunable platform to realize various correlated and topological phases, such as Mott insulators, unconventional uperconductivity and quantum anomalous Hall effect. Recently, the magic-angle twisted trilayer graphene (MATTG) has shown both robust superconductivity similar to magic-angle twisted bilayer graphene (MATBG) and other unique properties, including the Pauli-limit violating and re-entrant superconductivity. These rich properties are deeply roote…
It has recently been shown that quantum-confined states can appear in epitaxially grown van der Waals material heterobilayers without a rotational misalignment ($θ=0^\circ$), associated with flat bands in the Brillouin zone of the moiré pattern formed due to the lattice mismatch of the two layers. Peaks in the local density of states and confinement in a MoS$_2$/WSe$_2$ system was qualitatively described only considering local stacking arrangements, which cause band edge energies to vary spatially. In this work, we report the presence of large in-plane strain variation across the moiré unit ce…
We study the effects of heterostrain on moiré bands in twisted bilayer graphene and bilayer transition metal dichalcogenide (TMD) systems. For bilayer graphene with twist angle near $1^\circ$, we show that heterostrain significantly increases the energy separation between conduction and valence bands as well as the Dirac velocity at charge neutrality, which resolves several puzzles in scanning tunneling spectroscopy and quantum oscillation experiments at once. For bilayer TMD, we show that applying small heterostrain generally leads to flat moiré bands that are highly tunable.
We study the atomic and electronic structures of the commensurate double moiré superlattices in fully relaxed twisted bilayer graphene (TBG) nearly aligned with the hexagonal boron nitride (BN). The single-particle effective Hamiltonian ($\hat{H}^0$) taking into account the relaxation effect and the full moiré Hamiltonian introduced by BN has been built for TBG/BN. The mean-field (MF) band structures of the self-consistent Hartree-Fock (SCHF) ground states at different number ($ν$) of filled flat bands relative to the charge neutrality point (CNP) are obtained based on $\hat{H}^0$ in the plane…
The atomic structure at the interface between two-dimensional (2D) and three-dimensional (3D) materials influences properties such as contact resistance, photo-response, and high-frequency electrical performance. Moiré engineering is yet to be utilized for tailoring this 2D/3D interface, despite its success in enabling correlated physics at 2D/2D interfaces. Using epitaxially aligned MoS2/Au{111} as a model system, we demonstrate the use of advanced scanning transmission electron microscopy (STEM) combined with a geometric convolution technique in imaging the crystallographic 32 A moiré patter…
The flat bands resulting from moiré superlattices in magic-angle twisted bilayer graphene (MATBG) and ABC-trilayer graphene aligned with hexagonal boron nitride (ABC-TLG/hBN) have been shown to give rise to fascinating correlated electron phenomena such as correlated insulators and superconductivity. More recently, orbital magnetism associated with correlated Chern insulators was found in this class of layered structures centered at integer multiples of n0, the density corresponding to one electron per moiré superlattice unit cell. Here we report the experimental observation of ferromagnetism …
The valence band edge in tiny angle twist bilayers of MoS$_2$ and phosphorene is shown to consist of highly localized energy levels created by a `moiré quantum well', i.e. trapped by the interlayer moiré potential. These approximately uniformly spaced energy levels exhibit a richly modulated charge density, becoming ultra-localized at the valence band maximum. The number and spacing of such levels is controllable by the twist angle and interlayer interaction strength, suggesting the possibility of `moiré engineering' ordered arrays of quantum dots in 2d twist semi-conductors.
