Mean-field modeling of moiré materials: a user's guide with selected applications to twisted bilayer graphene

Growing twisted bilayer graphene at small angles

Frank-van der Merwe growth in bilayer graphene

Twisted bilayer graphene (TBG), which has drawn much attention in recent years, arises from van der Waals materials gathering each component together via van der Waals force. It is composed of two sheets of graphene rotated relatively to each other. Moiré potential, resulting from misorientation between layers, plays an essential role in determining the band structure of TBG, which directly relies on the twist angle. Once the twist angle approaches a certain critical value, flat bands will show up, indicating the suppression of kinetic energy, which significantly enhances the importance of Coulomb interaction between electrons. As a result, correlated states like correlated insulators emerge from TBG. Surprisingly, superconductivity in TBG is also reported in many experiments, which drags researchers into thinking about the underlying mechanism. Recently, the interest in the atomic reconstruction of TBG at small twist angles comes up and reinforces further understandings of properties of TBG. In addition, twisted multilayer graphene receives more and more attention, as they could likely outperform TBG although they are more difficult to handle experimentally. In this review, we mainly introduce theoretical and experimental progress on TBG. Besides the basic knowledge of TBG, we emphasize the essential role of atomic reconstruction in both experimental and theoretical investigations. The consideration of atomic reconstruction in small-twist situations can provide us with another aspect to have an insight into physical mechanism in TBG. In addition, we cover the recent hot topic, twisted multilayer graphene. While the bilayer situation can be relatively easy to resolve, multilayer situations can be really complicated, which could foster more unique and novel properties. Therefore, in the end of the review, we look forward to future development of twisted multilayer graphene.

How Magical Is Magic-Angle Graphene?

Controlling the balance between piezoelectric and flexoelectric effects is crucial for tailoring the electromechanical responses of a material. In twisted graphene, it is found that the electromechanical response near the domain walls (DWs) is dominated by either the flexoelectric effect as in twisted bilayer graphene (tBLG) or the piezoelectric effect as in twisted monolayer–bilayer graphene (tMBG). The codominance of both effects in a single system is rare. Here, utilizing lateral piezoresponse force microscopy (LPFM), we show that piezoelectric and flexoelectric effects can coexist and are equally important in twisted double bilayer graphene (tDBG), termed as the piezo-flexoelectric effect. Unlike tBLG and tMBG, distinctive two-step LPFM spatial profiles are captured across the moiré DWs of tDBG. By decomposing the LPFM signal into axisymmetric and antisymmetric components, we find that the angular dependence of both components satisfies sinusoidal relations. Quantitatively, the in-plane piezoelectric coefficient of DWs in tDBG is determined to be 0.15 pm/V by dual AC resonance tracking (DART) LPFM measurement. The conclusion is further supported by continuum mechanics simulations. Our results demonstrate that the stacking configuration serves as a powerful tuning knob for modulating the electromechanical responses of twisted van der Waals materials.

Bilayer graphene has been widely studied in recent years due to its intriguing physical properties and potential engineering applications. Here, we report on the stability measurements of isotope-labeled bilayer graphene with different stacking sequences. The results showed evidence of different defect intensity after the Ar plasma treatment. We found that the AB stacked bilayer graphene shows better stability when compared to twisted bilayer and monolayer graphene. However, for the protection of the under layer graphene, the twisted bilayer graphene showed better results. Our work demonstrates that the stability of bilayer graphene strongly depends on the layer stacking sequence.

Synthesis of Large-Area Single-Crystal Graphene

We study the magneto-optical conductivity of a number of van der Waals heterostructures, namely, twisted bilayer graphene, AB–AB and AB–BA stacked twisted double bilayer graphene and monolayer graphene and AB-stacked bilayer graphene on hexagonal boron nitride. As the magnetic field increases, the absorption spectrum exhibits a self-similar recursive pattern reflecting the fractal nature of the energy spectrum. Whilst twisted bilayer graphene displays only weak circular dichroism, the other four structures display strong circular dichroism with monolayer graphene and AB-stacked bilayer graphene on hexagonal boron nitride being particularly pronounced owing to strong inversion symmetry breaking properties of the hexagonal boron nitride layer. As the left and right circularly polarized light interact with these structures differently, plane-polarized incident light undergoes a Faraday rotation and gains an ellipticity when transmitted. The size of the respective angles is on the order of a degree.

Moiré superlattices of 2D materials with a small twist angle are thought to exhibit appreciable flexoelectric effect, though unambiguous confirmation of their flexoelectricity is challenging due to artifacts associated with commonly used piezoresponse force microscopy (PFM). For example, unexpectedly small phase contrast (≈8°) between opposite flexoelectric polarizations is reported in twisted bilayer graphene (tBG), though theoretically predicted value is 180°. Here a methodology is developed to extract intrinsic moiré flexoelectricity using twisted double bilayer graphene (tDBG) as a model system, probed by lateral PFM. For small twist angle samples, it is found that a vectorial decomposition is essential to recover the small intrinsic flexoelectric response at domain walls from a large background signal. The obtained threefold symmetry of commensurate domains with significant flexoelectric response at domain walls is fully consistent with the theoretical calculations. Incommensurate domains in tDBG with relatively large twist angles can also be observed by this technique. A general strategy is provided here for unraveling intrinsic flexoelectricity in van der Waals moiré superlattices while providing insights into engineered symmetry breaking in centrosymmetric materials.

This study has investigated the adsorption of phosphine toxic gas molecule on monolayer graphene, bilayer graphene and twisted bilayer graphene with, and without Magnesium impurity. The results of absorption energy studies using density functional theory (DFT) showed that bilayer graphene provides better adsorption than monolayer graphene and a difference in adsorption energy will be observed for twisted bilayer graphene with a rotation angle of 21.78°. By adding Mg impurity to the configurations, the sensitivity, and working temperature of the twisted bilayer graphene with Mg impurity increase compared to twisted bilayer graphene. Also, working temperature, and value of adsorption energy were calculated for bilayer graphene with Mg impurity less than Mg-doped twisted bilayer graphene, and monolayer graphene with Mg impurity.

Moiré is More: Access to New Properties of Two-Dimensional Layered Materials

Thanks to the recent discovery on the magic-angle bilayer graphene, twistronics is quickly becom11 ing a burgeoning field in condensed matter physics. This letter expands the realm of twistronics to acoustics by introducing twisted bilayer phononic graphene, which remarkably also harbors the magic angle, evidenced by the associated ultra-flat bands. Beyond mimicking quantum mechanical behaviors of twisted bilayer graphene, we show that their acoustic counterpart offers a considerably more straightforward and robust way to alter the interlayer hopping strength, enabling us to unlock magic angles (> 3 degrees) inaccessible in classical twisted bilayer graphene. This study, not only establishes the acoustical analog of twisted (magic-angle) bilayer graphene, providing a testbed more easily accessible to probe the interaction and misalignment between stacked 2D materials, but also points out the direction to a new phononic crystal design paradigm that could benefit applications such as enhanced acoustic emission and sensing.

The phenomenon of Rabi oscillations far from resonance is described in bilayer and few-layer graphene. These oscillations in the population and polarization at the Dirac point in n-layer graphene are seen in the nth harmonic term in the external driving frequency. The underlying reason behind these oscillations is attributable to the pseudospin degree of freedom possessed by all these systems. Conventional Rabi oscillations, which occur only near resonance, are seen in multiple harmonics in multilayer graphene. However, the experimentally measurable current density exhibits anomalous behaviour only in the first harmonic in all the graphene systems. A fully numerical solution of the optical Bloch equations is in complete agreement with the analytical results, thereby justifying the approximation schemes used in the latter. The same phenomena are also described in twisted bilayer graphene with and without an electric potential difference between the layers. It is found that the anomalous Rabi frequency is strongly dependent on twist angle for weak applied fields – a feature absent in single-layer graphene, whereas the conventional Rabi frequency is relatively independent of the twist angle.

It has been shown that the Kohn‒Luttinger superconductivity mechanism interplaying with other types of ordering can be implemented in systems with a hexagonal lattice. A number of unusual properties of such systems in the normal phase have also been considered. Our previous results on Kohn‒Luttinger superconductivity with p, d-, and f-wave pairing in monolayer and AB bilayer graphene, obtained disregarding the effect of substrate potential and impurities, have been presented in the first part. Then, the interplay of the superconducting Kohn‒Luttinger state with the spin density wave state in actual AB, AA, and twisted bilayer graphene has been discussed in detail. In the last parts, a number of anomalous properties in the normal phase and the appearance of nematic superconductivity alongside with the spin density wave in the twisted bilayer graphene have been presented.

Real-space tight-binding model for twisted bilayer graphene based on mapped Wannier functions