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It is shown that chiral plasmons, characterized by a longitudinal magnetic moment accompanying the longitudinal charge plasmon, lead to electromagnetic near-fields that are also chiral. For twisted bilayer graphene, we estimate that the near-field chirality of screened plasmons can be several orders of magnitude larger than that of the related circularly polarized light. The chirality also manifests itself in a deflection angle that is formed between the direction of the plasmon propagation and its Poynting vector. Twisted van der Waals heterostructures might thus provide a novel platform to promote enantiomer-selective physio-chemical processes in chiral molecules without the application of a magnetic field or external nanopatterning that break time-reversal, mirror plane, or inversion symmetry, respectively.

In the magic-angle twisted bilayer graphene (MA-TBG), strong electron-electron (e-e) correlations caused by the band-flattening lead to many exotic quantum phases such as superconductivity, correlated insulator, ferromagnetism, and quantum anomalous Hall effects, when its low-energy van Hove singularities (VHSs) are partially filled. Here our high-resolution scanning tunneling microscope and spectroscopy measurements demonstrate that the e-e correlation in a nonmagic-angle TBG with a twist angle θ = 1.49° still plays an important role in determining its electronic properties. Our most interesting observation on that sample is when one of its VHSs is partially filled, the one associated peak in the spectrum splits into four peaks. Simultaneously, the spatial symmetry of electronic states around the split VHSs is broken by the e-e correlation. Our analysis based on the continuum model suggests that such a one-to-four split of the VHS originates from the formation of an interaction-driven spin-valley-polarized metallic state near the VHS, which is a symmetry-breaking phase that has not been identified in the MA-TBG or in other systems.

Localized electrons subject to applied magnetic fields can restart to propagate freely through the lattice in delocalized magnetic Bloch states (MBSs) when the lattice periodicity is commensurate with the magnetic length. Twisted graphene superlattices with moiré wavelength tunability enable experimental access to the unique delocalization in a controllable fashion. Here, we report the observation and characterization of high-temperature Brown-Zak (BZ) oscillations which come in two types, 1/ B and B periodicity, originating from the generation of integer and fractional MBSs, in the twisted bilayer and trilayer graphene superlattices, respectively. Coexisting periodic-in-1/ B oscillations assigned to different moiré wavelengths are dramatically observed in small-angle twisted bilayer graphene, which may arise from angle-disorder-induced in-plane heteromoiré superlattices. Moreover, the vertical stacking of heteromoiré supercells in double-twisted trilayer graphene results in a mega-sized superlattice. The exotic superlattice contributes to the periodic-in- B oscillation and dominates the magnetic Bloch transport.

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°. From the spatial extension of the AA regions and the width of the flat bands, we estimate that many-body interactions in these systems are stronger than in twisted bilayer graphene. Chiral collapsed carbon nanotubes stand out as promising candidates to explore many-body effects and superconductivity in low dimensions, emerging as the one-dimensional analogues of twisted bilayer graphene.

Assembling monolayers into a bilayer system unlocks the rotational free degree of van der Waals (vdW) homo/heterostructure, enabling the building of twisted bilayer graphene (tBLG) which possesses novel electronic, optical, and mechanical properties. Previous methods for preparation of homo/heterstructures inevitably leave the polymer residue or hexagonal boron nitride ( h -BN) mask, which usually obstructs the measurement of intrinsic mechanical and surface properties of tBLG. Undoubtedly, to fabricate the designable tBLG with clean interface and surface is necessary but challenging. Here, we propose a simple and handy method to prepare atomically clean twisted bilayer graphene with controllable twist angles based on wetting-induced delamination. This method can transfer tBLG onto a patterned substrate, which offers an excellent platform for the observation of physical phenomena such as relaxation of moiré pattern in marginally tBLG. These findings and insight should ultimately guide the designable packaging and atomic characterization of the two-dimensional (2D) materials.

Recently twisted bilayer graphene (t-BLG) has emerged as a strongly correlated physical platform. Besides the apparent significance of band flatness, band topology may be another critical element in t-BLG and yet receives much less attention. Here we report the compelling evidence for nontrivial noninteracting Moiré band topology in t-BLG through a systematic nonlocal transport study and a K -theory examination. The nontrivial topology manifests itself as two pronounced nonlocal responses in the electron and hole superlattice gaps. We show that the nonlocal responses are robust to the twist angle and edge termination, exhibiting a universal scaling law. We elucidate that, although Berry curvature is symmetry-trivialized, two nontrivial Z 2 invariants characterize the Moiré Dirac bands, validating the topological origin of the observed nonlocal responses. Our findings not only provide a new perspective for understanding the strongly correlated t-BLG but also suggest a potential strategy to achieve topological metamaterials from trivial vdW materials.

We report a combined nano-photocurrent and infrared nanoscopy study of twisted bilayer graphene (TBG) enabling access to the local electronic phenomena at length scales as short as 20 nm. We show that the photocurrent changes sign at carrier densities tracking the local superlattice density of states of TBG. We use this property to identify domains of varying local twist angle by local photothermoelectric effect. Consistent with the photocurrent study, infrared nanoimaging experiments reveal optical conductivity features dominated by twist-angle-dependent interband transitions. Our results provide a fast and robust method for mapping the electronic structure of TBG and suggest that similar methods can be broadly applied to probe electronic inhomogeneities of Moiré superlattices in other van der Waals heterostructures.

The artificial stacking of atomically thin crystals suffers from intrinsic limitations in terms of control and reproducibility of the relative orientation of exfoliated flakes. This drawback is particularly severe when the properties of the system critically depends on the twist angle, as in the case of the dodecagonal quasicrystal formed by two graphene layers rotated by 30°. Here we show that large-area 30°-rotated bilayer graphene can be grown deterministically by chemical vapor deposition on Cu, eliminating the need of artificial assembly. The quasicrystals are easily transferred to arbitrary substrates and integrated in high-quality hexagonal boron nitride-encapsulated heterostructures, which we process into dual-gated devices exhibiting carrier mobility up to 10 5 cm 2 /(V s). From low-temperature magnetotransport, we find that the graphene quasicrystals effectively behave as uncoupled graphene layers, showing 8-fold degenerate quantum Hall states. This result indicates that the Dirac cones replica detected by previous photoemission experiments do not contribute to the electrical transport.

Stacking order has a strong influence on the coupling between the two layers of twisted bilayer graphene (BLG), which in turn determines its physical properties. Here, we report the investigation of the interlayer coupling of the epitaxially grown single-crystal 30°-twisted BLG on Cu(111) at the atomic scale. The stacking order and morphology of BLG is controlled by a rationally designed two-step growth process, that is, the thermodynamically controlled nucleation and kinetically controlled growth. The crystal structure of the 30°-twisted bilayer graphene (30°-tBLG) is determined to have quasicrystal-like symmetry. The electronic properties and interlayer coupling of the 30°-tBLG are investigated using scanning tunneling microscopy and spectroscopy. The energy-dependent local density of states with in situ electrostatic doping shows that the electronic states in two graphene layers are decoupled near the Dirac point. A linear dispersion originated from the constituent graphene monolayers is discovered with doubled degeneracy. This study contributes to controlled growth of twist-angle-defined BLG and provides insights on the electronic properties and interlayer coupling in this intriguing system.

We explore a network of electronic quantum valley Hall states in the moiré crystal of minimally twisted bilayer graphene. In our transport measurements, we observe Fabry-Pérot and Aharanov-Bohm oscillations that are robust in magnetic fields ranging from 0 to 8 T, which is in strong contrast to more conventional two-dimensional systems where trajectories in the bulk are bent by the Lorentz force. This persistence in magnetic field and the linear spacing in density indicate that charge carriers in the bulk flow in topologically protected, one-dimensional channels. With this work, we demonstrate coherent electronic transport in a lattice of topologically protected states.

We report a comprehensive study on the design of two-dimensional graphene-diamond nanocomposite superstructures formed through interlayer covalent bonding of twisted bilayer graphene with commensurate bilayers. The interlayer bonding is induced by patterned hydrogenation that leads to the formation of superlattices of two-dimensional nanodiamond domains embedded between the two graphene layers. We generalize a rigorous algorithm for the formation of all possible classes of these superstructures: the structural parameters employed to design such carbon nanocomposites include the commensurate bilayer's twist angle, the stacking type of the nanodomains where the interlayer bonds are formed, the interlayer bond pattern, and the interlayer C-C bond density that is proportional to the concentration of sp 3 -hybridized interlayer-bonded C atoms. We also analyze systematically the mechanical behavior of these nanocomposite superstructures on the basis of molecular-dynamics simulations of uniaxial tensile straining tests according to a reliable interatomic bond-order potential. We identify a range of structural parameters over which the fracture of these superstructures is ductile, mediated by void formation, growth, and coalescence, contrary to the typical brittle fracture of graphene. We introduce a ductility metric as an order parameter for the brittle-to-ductile transition, demonstrate its direct dependence on the fraction of sp 3 -hybridized interlayer-bonded C atoms, and show that increasing the fraction of interlayer-bonded C atoms beyond a critical level in certain classes of these superstructures induces their ductile mechanical response.

Twisted bilayer graphene (tBLG) with van Hove Singularity (VHS) has exhibited novel twist-angle-dependent chemical and physical phenomena. However, scalable production of high-quality tBLG is still in its infancy, especially lacking the angle controlled preparation methods. Here, we report a facile approach to prepare tBLG with large domain sizes (>100 μm) and controlled twist angles by a clean layer-by-layer transfer of two constituent graphene monolayers. The whole process without interfacial polymer contamination in two monolayers guarantees the interlayer interaction of the π-bond electrons, which gives rise to the existence of minigaps in electronic structures and the consequent formation of VHSs in density of state. Such perturbation on band structure was directly observed by angle-resolved photoemission spectroscopy with submicrometer spatial resolution (micro-ARPES). The VHSs lead to a strong light-matter interaction and thus introduce ∼20-fold enhanced intensity of Raman G-band, which is a characteristic of high-quality tBLG. The as-prepared tBLG with strong light-matter interaction was further fabricated into high-performance photodetectors with selectively enhanced photocurrent generation (up to ∼6 times compared with monolayer in our device).

Twisted bilayer graphene (tBLG) exhibits van Hove singularities (VHSs) in the density of states that can be tuned by changing the twist angle (θ), sparking various novel physical phenomena. Much effort has been devoted to investigate the θ-dependent physical properties of tBLG. Yet, the chemical properties of tBLG with VHSs, especially the chemical reactivity, remain unexplored. Here we report the first systematic study on the chemistry of tBLG through the photochemical reaction between graphene and benzoyl peroxide. Twisted bilayer graphene exhibits θ-dependent reactivity, and remarkably enhanced reactivity is obtained when the energy of incident laser matches with the energy interval of the VHSs of tBLG. This work provides an insight on the chemistry of tBLG, and the successful enhancement of chemical reactivity derived from VHS is highly beneficial for the controllable chemical modification of tBLG as well as the development of tBLG based devices.

Twisted bilayer graphene (tBLG) devices with ion gel gate dielectrics are studied using Raman spectroscopy in the twist angle regime where a resonantly enhanced G band can be observed. We observe prominent splitting and intensity quenching on the G Raman band when the carrier density is tuned away from charge neutrality. This G peak splitting is attributed to asymmetric charge doping in the two graphene layers, which reveals individual phonon self-energy renormalization of the two weakly coupled layers of graphene. We estimate the effective interlayer capacitance at low doping density of tBLG using an interlayer screening model. The anomalous intensity quenching of both G peaks is ascribed to the suppression of resonant interband transitions between the two saddle points (van Hove singularities) that are displaced in the momentum space by gate-tuning. In addition, we observe a softening (hardening) of the R Raman band, a superlattice-induced phonon mode in tBLG, in electron (hole) doping. Our results demonstrate that gate modulation can be used to control the optoelectronic and vibrational properties in tBLG devices.