ABC Trilayer Research Articles

Tunneling in ABC trilayer graphene superlattice

Tunneling in ABC trilayer graphene superlattice

Electron/infrared-phonon coupling in ABC trilayer graphene

Stacking order plays a crucial role in determining the crystal symmetry and has significant impacts on electronic, optical, magnetic, and topological properties. Electron-phonon coupling, which is central to a wide range of intriguing quantum phenomena, is expected to be intricately connected with stacking order. Understanding the stacking order-dependent electron-phonon coupling is essential for understanding peculiar physical phenomena associated with electron-phonon coupling, such as superconductivity and charge density waves. In this study, we investigate the effect of stacking order on electron-infrared phonon coupling in graphene trilayers. By using gate-tunable Raman spectroscopy and excitation frequency-dependent near-field infrared nanoscopy, we show that rhombohedral ABC-stacked trilayer graphene has a significant electron-infrared phonon coupling strength. Our findings provide novel insights into the superconductivity and other fundamental physical properties of rhombohedral ABC-stacked trilayer graphene, and can enable nondestructive and high-throughput imaging of trilayer graphene stacking order using Raman scattering.

Behavior of localized states in double twisted ABC trilayer graphene

We show that a double-twisted ABC trilayer graphene, formed by stacking two ABC trilayers with a rotation angle between them, is a semiconductor with a gap of about 30 meV. Importantly, flat bands in the electronic structure are observed even for large angles, and the localization of electrons follows the same pattern as in ABC trilayer graphene. Our first-principles calculations show that this behavior holds at least for rotation angles from 7 to 21 degrees. We further study the charge redistribution as a function of the angle. Below two degrees, the charge escapes from the rotated layers and AA zones, moving to the outer layers. This behavior is general for any ABA trilayer with one of the outer layers twisted (ABT). Our findings shed light on some peculiarities of rotated graphene, explaining the absence of a superconductivity phase on these double-trilayer and ABT systems.

Spin and orbital metallic magnetism in rhombohedral trilayer graphene

We provide a complete theoretical interpretation of the metallic broken spin/valley symmetry states recently discovered in ABC trilayer graphene (ABC) perturbed by a large transverse displacement field. Our conclusions combine insights from ABC trilayer graphene electronic structure models and mean field theory, and are guided by precise magneto-oscillation Fermi-surface-area measurements. We conclude that the physics of ABC trilayer graphene is shaped by the principle of momentum-space condensation, which favors Fermi surface reconstructions enabled by broken spin/valley flavor symmetries when the single-particle bands imply thin annular Fermi seas. We find one large outer Fermi surface enclosed majority-flavor states and one or more small inner hole-like Fermi surfaces enclosed minority-flavor states that are primarily responsible for nematic order. The smaller surfaces can rotate along a ring of van-Hove singularities or reconstruct into multiple Fermi surfaces with little cost in energy. We propose that the latter property is responsible for the quantum oscillation frequency fractionalization seen experimentally in some regions of the carrier-density/displacement-field phase diagram.

Quick identification of ABC trilayer graphene at nanoscale resolution via a near-field optical route

ABC-stacked trilayer graphene has exhibited a variety of correlated phenomena owing to its relatively flat bands and gate-tunable bandgap. However, convenient methods are still lacking for identifying ABC graphene with nanometer-scale resolution. Here we demonstrate that the scanning near-field optical microscope working in ambient conditions can provide quick recognition of ABC trilayer graphene with no ambiguity and excellent resolution (∼20 nm). The recognition is based on the difference in their near-field infrared (IR) responses between the ABA and ABC trilayers. We show that in most frequencies, the response of the ABC trilayer is weaker than the ABA trilayer. However, near the graphene phonon frequency (∼1585 cm−1), ABC’s response increases dramatically when gated and exhibits a narrow and sharp Fano-shape resonant line, whereas the ABA trilayer is largely featherless. Consequently, the IR contrast between ABC and ABA becomes reversed and can even be striking (ABC/ABA ∼ 3) near the graphene phonon frequency. The observed near-field IR features can serve as a golden rule to quickly distinguish ABA and ABC trilayers with no ambiguity, which could largely advance the exploration of correlation physics in ABC-stacked trilayer graphene.

Mott correlations in ABC graphene trilayer aligned with hBN

ABC trilayer graphene aligned with hexagonal boron nitride (ABC/hBN) and other moir\'e systems have shown insulating phases at integer fillings of the moir\'e lattice. The role of Mott physics in these insulating states has been questioned by observations of correlated states in a nonaligned ABC trilayer, but recent photocurrent experiments in aligned samples are consistent with the existence of a Mott insulating state at half filling. Using dynamical mean-field theory we address the effect of Mott correlations in ABC/hBN. We show that, at experimentally relevant interaction values, the electronic states are strongly affected by a significant spectral weight transfer not present without alignment to hBN. This effect, which emerges at interactions considerably smaller than ${U}_{\mathrm{Mott}}$ (at which the Mott metal-insulator transition takes place) and does not require symmetry breaking, also impacts the electronic properties at temperatures above the ordering transitions producing anomalous temperature and doping dependencies. Close to the Mott transition, the intramoir\'e unit cell interactions promote an antiferromagnetic state, probably breaking the ${C}_{3}$ symmetry, that would compete with the ferromagnetic exchange interactions to determine the ground state.

Competing orders and cascade of degeneracy lifting in doped Bernal bilayer graphene

Motivated by recent experiments [H. Zhou et al., Science 375, 774 (2022) and S. C. de la Barrera et al., arXiv:2110.13907], here we propose a general mechanism for valley and/or spin degeneracy lifting of the electronic bands in doped Bernal bilayer graphene, subject to electric displacement ($D$) fields. A $D$-field induced layer polarization (LP), when accompanied by a Hubbard repulsion-driven layer antiferromagnet (LAF) and next-nearest-neighbor repulsion-driven quantum anomalous Hall (QAH) orders, lifts the fourfold degeneracy of electronic bands, yielding a quarter metal for small doping, as also observed in ABC trilayer graphene. With the disappearance of the QAH order, electronic bands recover twofold valley degeneracy, thereby forming a conventional or compensated (with majority and minority carriers) half metal at moderate doping, depending on the relative strength of LP and LAF. At even higher doping and for a weak $D$ field only LAF survives and the Fermi surface recovers fourfold degeneracy. We also show that a pure repulsive electronic interaction mediated triplet $f$-wave pairing emerges from a parent correlated nematic liquid or compensated half metal when an in-plane magnetic field is applied to the system.

Proximity spin-orbit and exchange coupling in ABA and ABC trilayer graphene van der Waals heterostructures

We investigate the proximity spin-orbit and exchange couplings in ABA and ABC trilayer graphene encapsulated within monolayers of semiconducting transition-metal dichalcogenides and the ferromagnetic semiconductor Cr$_2$Ge$_2$Te$_6$. Employing first-principles calculations we obtain the electronic structures of the multilayer stacks and extract the relevant proximity-induced orbital and spin interaction parameters by fitting the low-energy bands to model Hamiltonians. We also demonstrate the tunability of the proximity effects by a transverse electric field. Using the model Hamiltonians we also study mixed spin-orbit/exchange coupling encapsulation, which allows to tailor the spin interactions very efficiently by the applied field. We also summarize the spin-orbit physics of bare ABA, ABC, and ABB trilayers, and provide, along with the first-principles results of the electronic band structures, density of states, spin splittings, and electric-field tunabilities of the bands, qualitative understanding of the observed behavior and realistic model parameters as a resource for model simulations of transport and correlation physics in trilayer graphene.

Flat bands, electron interactions, and magnetic order in magic-angle mono-trilayer graphene

Starting with twisted bilayer graphene, graphene-based moir\'e materials have recently been established as a new platform for studying strong electron correlations. In this paper, we study twisted graphene monolayers on trilayer graphene and demonstrate that this system can host flat bands when the twist angle is close to the magic angle of $1.{16}^{\ensuremath{\circ}}$. When monolayer graphene is twisted on ABA trilayer graphene, the flat bands are not isolated, but are intersected by a Dirac cone with a large Fermi velocity. In contrast, graphene twisted on ABC trilayer graphene (denoted AtABC) exhibits a gap between flat and remote bands. Since ABC trilayer graphene and twisted bilayer graphene are known to host broken-symmetry phases, we further investigate the ostensibly similar magic-angle AtABC system. We study the effect of electron-electron interactions in AtABC using both Hartree theory and an atomic Hubbard theory to calculate the magnetic phase diagram as a function of doping, twist angle, and perpendicular electric field. Our analysis reveals a rich variety of magnetic orderings, including ferromagnetism and ferrimagnetism, and demonstrates that a perpendicular electric field makes AtABC more susceptible to magnetic ordering.

Evidence for Moiré Trions in Twisted MoSe2 Homobilayers.

Moiré superlattices of van der Waals structures offer a powerful platform for engineering band structure and quantum states. For instance, Moiré superlattices in magic-angle twisted bilayer graphene, ABC trilayer graphene have been shown to harbor correlated insulating and superconducting states, while in transition metal dichalcogenide (TMD) twisted bilayers, Moiré excitons have been identified. Here we show that the effects of a Moiré superlattice on the band structure are general: In TMD twisted bilayers, excitons and exciton complexes can be trapped in the superlattice in a manner analogous to ultracold bosonic or Fermionic atoms in optical lattices. Using twisted MoSe2 homobilayers as a model system, we present evidence for Moiré trions. Our results thus open possibilities for designer van der Waals structures hosting arrays of Fermionic or bosonic quasiparticles, which can be used to realize tunable many-body states crucial for quantum simulation and quantum information processing.

Quantum Hall spin liquids and their possible realization in moiré systems

Recently, Chern insulators with Chern numbers $C=1$ and 2 in zero (or very small) magnetic field have been observed in two moire graphene systems: twisted bilayer graphene and ABC trilayer graphene, both aligned with a hexagonal boron-nitride (h-BN) substrate. These Chern insulator states arise due to many-body effects in the Chern bands of these systems when they are partially filled to a total integer filling ${\ensuremath{\nu}}_{T}=1,3$ (including spin and valley degrees of freedom). A simple possible explanation is from Hartree-Fock mean-field theory which predicts valley and spin polarization in the zero bandwidth limit, similar to the ``quantum Hall ferromagnetism'' in Landau levels. Though valley polarization is implied by the existing experiments, the fate of the spin degree of freedom is not presently clear. In this paper, we propose alternative valley polarized---but not spin polarized---candidates for the observed QAH effect. For a valley polarized spinful Chern band at filling ${\ensuremath{\nu}}_{T}=1$, we describe a class of exotic Chern insulator phases through spin-charge separation: charge is in a conventional Chern insulator phase with quantized Hall conductivity, while the spin forms disordered spin liquid phase with fractionalization, which we dub quantum Hall spin liquids. We construct a simple class of ${Z}_{2}$ quantum Hall spin liquid as analogs of the familiar ${Z}_{2}$ spin liquid through slave fermion-Schwinger boson parton theory. Condensation of the spinon from the ${Z}_{2}$ quantum Hall spin liquid can lead to a quantum Hall antiferromagnet which is yet another, less exotic, candidate for the experimentally observed Chern insulator. We offer several experimental proposals to probe the quantum Hall spin liquid and the quantum Hall antiferromagnetic phases. We briefly comment on the generalization to the filling ${\ensuremath{\nu}}_{T}=2$ and propose possible quantum valley Hall spin liquid without full spin polarization. Finally, we also propose another class of QHSL using fermionic spinons, including phases supporting non-Abelian anyons.

Pairing in graphene-based moiré superlattices

We present a systematic classification and analysis of possible pairing instabilities in graphene-based moir\'e superlattices. Motivated by recent experiments on twisted double-bilayer graphene showing signs of triplet superconductivity, we analyze both singlet and triplet pairing separately, and describe how these two channels behave close to the limit where the system is invariant under separate spin rotations in the two valleys, realizing an SU(2)$_+$ $\times$ SU(2)$_-$ symmetry. Further, we discuss the conditions under which singlet and triplet can mix via two nearly degenerate transitions, and how the different pairing states behave when an external magnetic field is applied. The consequences of the additional microscopic or emergent approximate symmetries relevant for superconductivity in twisted bilayer graphene and ABC trilayer graphene on hexagonal boron nitride are described in detail. We also analyze which of the pairing states can arise in mean-field theory and study the impact of corrections coming from ferromagnetic fluctuations. For instance, we show that, close to the parameters of mean-field theory, a nematic mixed singlet-triplet state emerges. Our study illustrates that graphene superlattices provide a rich platform for exotic superconducting states, and allow for the admixture of singlet and triplet pairing even in the absence of spin-orbit coupling.

Ferromagnetism in Narrow Bands of Moiré Superlattices.

Many graphene moiré superlattices host narrow bands with nonzero valley Chern numbers. We provide analytical and numerical evidence for a robust spin and/or valley polarized insulator at total integer band filling in nearly flat bands of several different moiré materials. In the limit of a perfectly flat band, we present analytical arguments in favor of the ferromagnetic state substantiated by numerical calculations. Further, we numerically evaluate its stability for a finite bandwidth. We provide exact diagonalization results for models appropriate for ABC trilayer graphene aligned with hBN, twisted double bilayer graphene, and twisted bilayer graphene aligned with hBN. We also provide DMRG results for a honeycomb lattice with a quasiflat band and nonzero Chern number, which extend our results to larger system sizes. We find a maximally spin and valley polarized insulator at all integer fillings when the band is sufficiently flat. We also show that interactions may induce effective dispersive terms strong enough to destabilize this state. These results still hold in the case of zero valley Chern number (for example, trivial side of TLG/hBN). We give an intuitive picture based on extended Wannier orbitals, and emphasize the role of the quantum geometry of the band, whose microscopic details may enhance or weaken ferromagnetism in moiré materials.

Mott and generalized Wigner crystal states in WSe2/WS2 moiré superlattices.

Moiré superlattices can be used to engineer strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states observed in magic-angle twisted-bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices1-4. Transition metal dichalcogenide moiré heterostructures provide another model system for the study of correlated quantum phenomena5 because of their strong light-matter interactions and large spin-orbit coupling. However, experimental observation of correlated insulating states in this system is challenging with traditional transport techniques. Here we report the optical detection of strongly correlated phases in semiconducting WSe2/WS2 moiré superlattices. We use a sensitive optical detection technique and reveal a Mott insulator state at one hole per superlattice site and surprising insulating phases at 1/3 and 2/3 filling of the superlattice, which we assign to generalized Wigner crystallization on the underlying lattice6-11. Furthermore, the spin-valley optical selection rules12-14 of transition metal dichalcogenide heterostructures allow us to optically create and investigate low-energy excited spin states in the Mott insulator. We measure a very long spin relaxation lifetime of many microseconds in the Mott insulating state, orders of magnitude longer than that of charge excitations. Our studies highlight the value of using moiré superlattices beyond graphene to explore correlated physics.

Large-area epitaxial growth of curvature-stabilized ABC trilayer graphene

The properties of van der Waals (vdW) materials often vary dramatically with the atomic stacking order between layers, but this order can be difficult to control. Trilayer graphene (TLG) stacks in either a semimetallic ABA or a semiconducting ABC configuration with a gate-tunable band gap, but the latter has only been produced by exfoliation. Here we present a chemical vapor deposition approach to TLG growth that yields greatly enhanced fraction and size of ABC domains. The key insight is that substrate curvature can stabilize ABC domains. Controllable ABC yields ~59% were achieved by tailoring substrate curvature levels. ABC fractions remained high after transfer to device substrates, as confirmed by transport measurements revealing the expected tunable ABC band gap. Substrate topography engineering provides a path to large-scale synthesis of epitaxial ABC-TLG and other vdW materials.

Spin liquids and pseudogap metals in the SU(4) Hubbard model in a moiré superlattice

Motivated by the realization of spin-valley Hubbard on triangular moir\'e superlattice in ABC trilayer graphene aligned with hexagon boron nitride (hBN) and possibly also in twisted transition metal dichalcogenide homobilayers, we study possible Mott insulating phases and pseudogap metals based on symmetry constraint and parton mean field theories. First we show that Luttinger constraint allows two distinct symmetric and featureless Fermi liquids when there is an inter-valley Hund's term breaking $SU(4)$ spin rotation. Especially, there exists a symmetric and featureless "pseudogap metal" with small Fermi surfaces. Then we suggest to search for such an unconventional metallic state by doping the Mott insulator at $\nu_T=2$. For this purpose, we study the $\nu_T=2$ Mott insulator using $SO(6)$ Schwinger boson or Schwinger fermion parton. At the $SU(4)$ symmetric point, we find two symmetric $Z_2$ spin liquids. With a large anti inter-valley Hund's term, a featureless Mott insulator is natural. Next we show that doping the featureless Mott insulator or a $Z_2$ spin liquid can lead to featureless or orthogonal "pseudogap metal" with small Fermi surfaces proportional to the doping. Besides, we also provide one scenario for the evolution from "pseudogap metal" to the conventional Fermi liquid through an intermediate exotic "deconfined metal" phase. Last, we give brief comments on the possibility of $U(1)$ spinon fermi surface state or $Z_4$ spin liquid at $\nu_T=1$.

Evidence of a gate-tunable Mott insulator in a trilayer graphene moiré superlattice

Mott insulator plays a central role in strongly correlated physics, where the repulsive Coulomb interaction dominates over the electron kinetic energy and leads to insulating states with one electron occupying each unit cell. Doped Mott insulator is often described by the Hubbard model3, which can give rise to other correlated phenomena such as unusual magnetism and even high-temperature superconductivity. A tunable Mott insulator, where the competition between the Coulomb interaction and the kinetic energy can be varied in situ, can provide an invaluable model system for the study of Mott physics. Here we report the realization of such a tunable Mott insulator in the ABC trilayer graphene (TLG) and hexagonal boron nitride (hBN) heterostructure with a moir\'e superlattice. Unlike massless Dirac electrons in monolayer graphene, electrons in pristine ABC TLG are characterized by quartic energy dispersion and large effective mass that are conducive for strongly correlated phenomena. The moir\'e superlattice in TLG/hBN heterostructures leads to narrow electronic minibands that are gate tunable. Each filled miniband contains 4 electrons in one moir\'e lattice site due to the spin and valley degeneracy of graphene. The Mott insulator states emerge at 1/4 and 1/2 fillings, corresponding to one electron and two electrons per site, respectively. Moreover, the Mott states in the ABC TLG/hBN heterostructure exhibit unprecedented tunability: the Mott gap can be modulated in situ by a vertical electrical field, and at the meantime, the electron doping can be gate-tuned to fill the band from one Mott insulating state to another. Our observation of a tunable Mott insulator opens up exciting opportunities to explore novel strongly correlated phenomena in two-dimensional moir\'e superlattice heterostructures.

Gate-Tunable Topological Flat Bands in Trilayer Graphene Boron-Nitride Moiré Superlattices.

We investigate the electronic structure of the flat bands induced by moiré superlattices and electric fields in nearly aligned ABC trilayer graphene (TLG) boron-nitride (BN) interfaces where Coulomb effects can lead to correlated gapped phases. Our calculations indicate that valley-spin resolved isolated superlattice flat bands that carry a finite Chern number C=3 proportional to the layer number can appear near charge neutrality for appropriate perpendicular electric fields and twist angles. When the degeneracy of the bands is lifted by Coulomb interactions, these topological bands can lead to anomalous quantum Hall phases that embody orbital and spin magnetism. Narrow bandwidths of ∼10 meV achievable for a continuous range of twist angles θ≲0.6° with moderate interlayer potential differences of ∼50 meV make the TLG-BN systems a promising platform for the study of electric-field tunable Coulomb-interaction-driven spontaneous Hall phases.

Topological properties of graphene moiré superlattice systems and recent optical studies

When 2D materials with different lattice constants or lattice rotation angles are stacked together, a periodic moiré pattern will appear. Such moiré superlattice introduces a new two dimensional periodic potential, which can greatly change the physical properties of the original systems. Recent experimental studies of moiré superlattices formed by graphene on graphene and graphene on hexagonal boron nitride have revealed very rich strong correlation effects and topological effects due to novel states in superlattice minibands. It has been shown that flat bands in graphene-based moiré superlattice systems can host both topological states and strongly correlated states, which can be controlled by an external electric field. In bilayer graphene, ABC stacked trilayer graphene and twisted bilayer-bilayer graphene, the number of valence and conduction bands near the Dirac point and even the band topology and bandwidth can be changed by varying the stacking angle between graphene layers or the applied bias voltage. Moreover, the competition between kinetic energy and coulomb interaction depends on the bandwidth and the external electric field, and at the so-called magic angle mott insulator states and superconductivity were observed. Twisted bilayer-bilayer graphene has also been predicted to show similar intriguing properties, including electrically tunable strongly correlated insulators, superconductivity and many rich topological states. In graphene-based moiré systems, the combination of topological states and strong correlations is expected to lead to a broad range of novel phenomena that are not achievable in other material systems. Therefore, graphene moiré systems is likely to bring substantial progress to the study of topological materials. In this paper, we review theoretical and experimental investigations of the topological properties of graphene moiré superlattices, including topological domain wall states in bilayer graphene and topological effects in twisted bilayer graphene, ABC trilayer graphene and twisted double bilayer graphene. The origins of topological properties of these systems are discussed as well as topological phenomena observed in various experiments. Finally, recent near-field optical studies of the band structure and novel topological properties of graphene moiré superlattices are discussed.

Selective fabrication of free-standing ABA and ABC trilayer graphene with/without Dirac-cone energy bands

Graphene is a single-layer carbon sheet with a honeycomb structure, and bilayer graphene consists of two graphene sheets with AB stacking. In trilayer graphene, the third graphene sheet has two possible stacking sequences, A or C, when it is overlaid on bilayer graphene. It has been theoretically predicted that trilayer graphene exhibits a variety of novel electronic properties with/without a Dirac-cone band, depending on the stacking sequence. In this regard, trilayer graphene has a high potential for widening the capability of graphene-based electronic devices. However, the difficulty of selective fabrication has hindered the progress of research. Here, we report the first success in the selective fabrication of quasi-free-standing trilayer graphene with ABA or ABC stacking grown epitaxially on hydrogen-terminated silicon carbide. Angle-resolved photoemission spectroscopy (ARPES) clearly demonstrated that our trilayer graphene with ABA stacking has a massless Dirac-like band near the Fermi level, while that with ABC stacking shows a parabolic non-Dirac-like band dispersion.