Twisted Trilayer Graphene Research Articles

Robust flat bands in twisted trilayer graphene moiré quasicrystals

Moiré structures formed by twisting three layers of graphene with two independent twist angles present an ideal platform for studying correlated quantum phenomena, as an infinite set of angle pairs is predicted to exhibit flat bands. Moreover, the two mutually incommensurate moiré patterns among the twisted trilayer graphene (TTG) can form highly tunable moiré quasicrystals. This enables us to extend correlated physics in periodic moiré crystals to quasiperiodic systems. However, direct local characterization of the structure of the moiré quasicrystals and of the resulting flat bands are still lacking, which is crucial to fundamental understanding and control of the correlated moiré physics. Here, we demonstrate the existence of flat bands in a series of TTGs with various twist angle pairs and show that the TTGs with different magic angle pairs are strikingly dissimilar in their atomic and electronic structures. The lattice relaxation and the interference between moiré patterns are highly dependent on the twist angles. Our direct spatial mappings, supported by theoretical calculations, reveal that the localization of the flat bands exhibits distinct symmetries in different regions of the moiré quasicrystals.

Effect of lattice relaxation on electronic spectra of helically twisted trilayer graphene: large-scale atomistic simulation approach

Effect of lattice relaxation on electronic spectra of helically twisted trilayer graphene: large-scale atomistic simulation approach

Tunable inter-moiré physics in consecutively twisted trilayer graphene

Tunable inter-moiré physics in consecutively twisted trilayer graphene

Nature of even and odd magic angles in helical twisted trilayer graphene

Nature of even and odd magic angles in helical twisted trilayer graphene

Pseudomagnetic fields in fully relaxed twisted bilayer and trilayer graphene

We present simple models to describe the in-plane and the out-of-plane lattice relaxation in twisted bilayer and symmetrically twisted trilayer graphene. Analytical results and series expansions show that for twist angles θ>1.4∘ , the in-plane atomic displacements lead to pseudomagnetic fields weakly dependent on θ. In symmetrically twisted trilayer graphene, the central layer in-plane relaxation is greatly enhanced. The joint effect of the relaxation-induced pseudoscalar potentials and the associated energy difference between interlayer dimer and non-dimer pairs resulted in a significant electron–hole asymmetry both in twisted bilayer and trilayer graphene.

Inhomogeneous and nonlocal optical response in magic-angle twisted trilayer graphene

Inhomogeneous and nonlocal optical response in magic-angle twisted trilayer graphene

Evolution from Bardeen–Cooper–Schrieffer to Bose–Einstein Condensation in Two Dimensions: Crossovers and Topological Quantum Phase Transitions

We review aspects of the evolution from Bardeen–Cooper–Schrieffer (BCS) to Bose–Einstein condensation (BEC) in two dimensions, which have now become relevant in systems with low densities, such as gated superconductors Li xZrNCl, magic-angle twisted trilayer graphene, FeSe, FeSe1− xS x, and ultracold Fermi superfluids. We emphasize the important role played by chemical potentials in determining crossovers or topological quantum phase transitions during the BCS–BEC evolution in one-band and two-band superfluids and superconductors. We highlight that crossovers from BCS to BEC occur for pairing in nonnodal s-wave channels, whereas topological quantum phase transitions, in which the order parameter symmetry does not change, arise for pairing in any nodal higher angular momentum channels, such as d-wave. We conclude by discussing a few open questions regarding the BCS-to-BEC evolution in 2D, including modulus fluctuations of the order parameter, tighter upper bounds on critical temperatures, and the exploration of lattice effects in two-band superconductors and superfluids.

Angle-resolved transport non-reciprocity and spontaneous symmetry breaking in twisted trilayer graphene.

The identification and characterization of spontaneous symmetry breaking is central to our understanding of strongly correlated two-dimensional materials. In this work, we utilize the angle-resolved measurements of transport non-reciprocity to investigate spontaneous symmetry breaking in twisted trilayer graphene. By analysing the angular dependence of non-reciprocity in both longitudinal and transverse channels, we are able to identify the symmetry axis associated with the underlying electronic order. We report that a hysteretic rotation in the mirror axis can be induced by thermal cycles and a large current bias, supporting the spontaneous breaking of rotational symmetry. Moreover, the onset of non-reciprocity with decreasing temperature coincides with the emergence of orbital ferromagnetism. Combined with the angular dependence of the superconducting diode effect, our findings uncover a direct link between rotational and time-reversal symmetry breaking. These symmetry requirements point towards exchange-driven instabilities in momentum space as a possible origin for transport non-reciprocity in twisted trilayer graphene.

Robust and reentrant superconductivity in magic-angle twisted trilayer graphene

Robust and reentrant superconductivity in magic-angle twisted trilayer graphene

Enhanced Electrochemical Activity Volcanoes in Flat-Band Twisted Trilayer Graphene

Electrochemical reactions at electrode-electrolyte interfaces are often controlled by modifying the substrate and thereby tuning the adsorption energy to reach peaks of activity volcanoes. In this work, we attempt to enhance interfacial charge transfer kinetics through modifying the electronic density of states of an electrode which offers highly tunable flat bands such as the twisted graphene system, allowing greater overlap with the redox couple states. Correspondingly, we develop a twist-dependent electrochemical activity map, combining a tight-binding electronic structure model with modified Marcus-Hush-Chidsey kinetics in trilayer graphene. We identify a counterintuitive rate enhancement region spanning the magic angle curve and incommensurate twists of the system geometry. At room temperature, we find a broad activity peak with a ruthenium hexamine redox couple in regions corresponding to both magic angles and incommensurate angles, a result qualitatively distinct from the twisted bilayer case. Flat bands and incommensurability offer new avenues for reaction rate enhancements in electrochemical transformations.

Imaging inter-valley coherent order in magic-angle twisted trilayer graphene.

Magic-angle twisted trilayer graphene (MATTG) exhibits a range of strongly correlated electronic phases that spontaneously break its underlying symmetries1,2. Here we investigate the correlated phases of MATTG using scanning tunnelling microscopy and identify marked signatures of interaction-driven spatial symmetry breaking. In low-strain samples, over a filling range of about two to three electrons or holes per moiré unit cell, we observe atomic-scale reconstruction of the graphene lattice that accompanies a correlated gap in the tunnelling spectrum. This short-scale restructuring appears as a Kekulé supercell-implying spontaneous inter-valley coherence between electrons-and persists in a wide range of magnetic fields and temperatures that coincide with the development of the gap. Large-scale maps covering several moiré unit cells further reveal a slow evolution of the Kekulé pattern, indicating that atomic-scale reconstruction coexists with translation symmetry breaking at a much longer moiré scale. We use auto-correlation and Fourier analyses to extract the intrinsic periodicity of these phases and find that they are consistent with the theoretically proposed incommensurate Kekulé spiral order3,4. Moreover, we find that the wavelength characterizing moiré-scale modulations monotonically decreases with hole doping away from half-filling of the bands and depends weakly on the magnetic field. Our results provide essential insights into the nature of the correlated phases of MATTG in the presence of strain and indicate that superconductivity can emerge from an inter-valley coherent parent state.

Magic angle butterfly in twisted trilayer graphene

Magic angle butterfly in twisted trilayer graphene

Hofstadter moiré butterfly in twisted trilayer graphene

Hofstadter moiré butterfly in twisted trilayer graphene

Interferometric Imaging of Twisted Trilayer Graphene Moiré Superlattices.

Interferometric Imaging of Twisted Trilayer Graphene Moiré Superlattices.

Anomalous Interfacial Electron-Transfer Kinetics in Twisted Trilayer Graphene Caused by Layer-Specific Localization.

Interfacial electron-transfer (ET) reactions underpin the interconversion of electrical and chemical energy. It is known that the electronic state of electrodes strongly influences ET rates because of differences in the electronic density of states (DOS) across metals, semimetals, and semiconductors. Here, by controlling interlayer twists in well-defined trilayer graphene moirés, we show that ET rates are strikingly dependent on electronic localization in each atomic layer and not the overall DOS. The large degree of tunability inherent to moiré electrodes leads to local ET kinetics that range over 3 orders of magnitude across different constructions of only three atomic layers, even exceeding rates at bulk metals. Our results demonstrate that beyond the ensemble DOS, electronic localization is critical in facilitating interfacial ET, with implications for understanding the origin of high interfacial reactivity typically exhibited by defects at electrode-electrolyte interfaces.

Ising superconductivity induced from spin-selective valley symmetry breaking in twisted trilayer graphene

We show that the e-e interaction induces a strong breakdown of valley symmetry for each spin channel in twisted trilayer graphene, leading to a ground state where the two spin projections have opposite sign of the valley symmetry breaking order parameter. This leads to a spin-valley locking in which the electrons of a Cooper pair are forced to live on different Fermi lines attached to opposite valleys. Furthermore, we find an effective intrinsic spin-orbit coupling explaining the protection of the superconductivity against in-plane magnetic fields. The effect of spin-selective valley symmetry breaking is validated as it reproduces the experimental observation of the reset of the Hall density at 2-hole doping. It also implies a breakdown of the symmetry of the bands from C6 to C3, with an enhancement of the anisotropy of the Fermi lines which is at the origin of a Kohn-Luttinger (pairing) instability. The isotropy of the bands is gradually recovered, however, when the Fermi level approaches the bottom of the second valence band, explaining why the superconductivity fades away in the doping range beyond 3 holes per moiré unit cell in twisted trilayer graphene.

Supermoiré low-energy effective theory of twisted trilayer graphene

Stacking three monolayers of graphene with a twist generally produces two moir\'e patterns. A moir\'e of moir\'e structure then emerges at larger distance where the three layers periodically realign. We devise here an effective low-energy theory to describe the spectrum at distances larger than the moir\'e lengthscale. In each valley of the underlying graphene, the theory comprises one Dirac cone at the ${\bf \Gamma}_M$ point of the moir\'e Brillouin zone and two weakly gapped points at ${\bf K}_M$ and ${\bf K}'_M$. The velocities and small gaps exhibit a spatial dependence in the moir\'e-of-moir\'e unit cell, entailing a non-abelian connection potential which ensures gauge invariance. The resulting model is numerically solved and a fully connected spectrum is obtained, which is protected by the combination of time-reversal and twofold-rotation symmetries.

Tunable Superconductivity and Möbius Fermi Surfaces in an Inversion-Symmetric Twisted van der Waals Heterostructure

We theoretically study a moiré superlattice geometry consisting of mirror-symmetric twisted trilayer graphene surrounded by identical transition metal dichalcogenide layers. We show that this setup allows us to switch on or off and control the spin-orbit splitting of the Fermi surfaces via application of a perpendicular displacement field D_{0} and explore two manifestations of this control: first, we compute the evolution of superconducting pairing with D_{0}; this features a complex admixture of singlet and triplet pairing and, depending on the pairing state in the parent trilayer system, phase transitions between competing superconducting phases. Second, we reveal that, with application of D_{0}, the spin-orbit-induced spin textures exhibit vortices which lead to "Möbius fermi surfaces" in the interior of the Brillouin zone: diabatic electron trajectories, which are predicted to dominate quantum oscillation experiments, require encircling the Γ point twice, making their Möbius nature directly observable. Further, we show that the superconducting order parameter inherits the unconventional, Möbius spin textures. Our findings suggest that this system provides a promising experimental avenue for systematically studying the impact of spin-orbit coupling on the multitude of topological and correlated phases in near-magic-angle twisted trilayer graphene.

Unravelling the magic of twisted trilayer graphene.

Unravelling the magic of twisted trilayer graphene.

Commensurate and incommensurate double moiré interference in twisted trilayer graphene

Twisted graphene multi-layers have been recently demonstrated to share several correlation-driven behaviours with twisted bilayer graphene. In general, the van Hove singularities (VHSs) can be used as a proxy of the tendency for correlated behaviours. In this paper, we adopt an atomistic method by combining tight-binding method with the semi-classical molecular dynamics to investigate the electronic structures of twisted trilayer graphene (TTG) with two independent twist angles. The two independent twist angles can lead to the interference of the moir\'e patterns forming a variety of commensurate/incommensurate complex supermoir\'e patterns. In particular, the lattice relaxation, twist angle and angle disorder effects on the VHS are discussed. We find that the lattice relaxation significantly influence the position and magnitude of the VHSs. In the supermoir\'e TTG, the moir\'e interference provides constructive or destructive effects depending on the relative twist angle. By modulating the two independent twist angles, novel superstructures, for instance, the Kagome-like lattice, could constructed via the moir\'e pattern. Moreover, we demonstrate that a slight change in twist angles (angle disorder) provides a significant suppression of the peak of the VHSs. Apart from the moir\'e length, the evolution of the VHSs and the LDOS mapping in real space could be used to identify the twist angles in the complicated TTG. In practice, our work could provide a guide for exploring the flat band behaviours in the supermoir\'e TTG experimentally.