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ABC-stacked rhombohedral graphene multilayers exhibit a wide variety of electronic ground states characterized by broken isospin symmetry and superconductivity. Recently, indirect evidence of inter-valley coherent (IVC) order has been reported in rhombohedral trilayer graphene (RTG), with possible implications for the origin of superconductivity. Here, we report the direct visualization of IVC order in RTG using scanning tunneling microscopy and spectroscopy. Tuning the chemical potential through the Van Hove singularity near the edge of the valence band, we observe a cascade of phase transitions associated with the formation of half- and quarter-metal states. IVC phases, distinguished by an enlarged real space unit cell, are directly imaged near both the high- and low-density boundaries of the half-metal phase. At high hole density, we precisely reconstruct the IVC band structure through quasiparticle interference. Intriguingly, the charge density modulations reveal a C3-symmetric incommensurate IVC order that agrees with the recent prediction of an IVC-crystal phase. Our findings demonstrate that IVC phases are a widespread symmetry-broken ground state within graphene systems., Comment: 22 pages, 4 figures

Inducing superconducting correlations in chiral edge states is predicted to generate topologically protected zero energy modes with exotic quantum statistics. Experimental efforts to date have focused on engineering interfaces between superconducting materials, typically amorphous metals, and semiconducting quantum Hall or quantum anomalous Hall (QAH) systems. However, the strong interfacial disorder inherent can prevent the formation of isolated topological modes. An appealing alternative is to use low-density flat band materials where the ground state can be tuned between intrinsic superconducting and quantum anomalous Hall states using only the electric field effect. However, quantized transport and superconductivity have not been simultaneously achieved. Here, we show that rhombohedral tetralayer graphene aligned to a hexagonal boron nitride substrate hosts a quantized anomalous Hall state at superlattice filling $\nu = -1$ as well as a superconducting state at $\nu \approx -3.1$ at zero magnetic field. Remarkably, gate voltage can also be used to actuate nonvolatile switching of the chirality in the quantum anomalous Hall state, allowing arbitrarily reconfigurable networks of topological edge modes in locally gated devices. Thermodynamic compressibility measurements further reveal a topologically ordered fractional Chern insulator at $\nu = 2/3$, also stable at zero magnetic field, enabling proximity coupling between superconductivity and fractionally charged edge modes. Finally, we show that integrating an additional transition metal dichalcogenide layer to the heterostructure enhances the maximum superconducting critical temperature and nucleates new superconducting pockets, while leaving the topology of $\nu = -1$ the quantum anomalous Hall state intact. Our results pave the way for hybrid interfaces between superconductors and topological edge states in the low-disorder limit.

Graphene and transition metal dichalcogenide flat-band systems show similar phase diagrams, replete with magnetic and superconducting phases. An abiding question has been whether magnetic ordering competes with superconductivity or facilitates pairing. The advent of crystalline graphene superconductors enables a new generation of controlled experiments to probe the microscopic origin of superconductivity. For example, recent studies of Bernal bilayer graphene show a dramatic increase in the observed domain and critical temperature $T_c$ of superconducting states in the presence of enhanced spin-orbit coupling; the mechanism for this enhancement, however, remains unclear. Here, we show that introducing spin-orbit coupling in rhombohedral trilayer graphene (RTG) via substrate proximity effect generates new superconducting pockets for both electron and hole doping, with maximal $T_c\approx$ 300mK three times larger than in RTG encapsulated by hexagonal boron nitride alone. Using local magnetometry and thermodynamic compressibility measurements, we show that superconductivity straddles an apparently continuous transition between a spin-canted state with a finite in-plane magnetic moment and a state with complete spin-valley locking. This transition is reproduced in our Hartree-Fock calculations, where it is driven by the competition between spin-orbit coupling and the carrier-density-tuned Hund's interaction. Our experiment suggests that the enhancement of superconductivity by spin-orbit coupling is driven not by a change in the ground state symmetry or degeneracy but rather by a quantitative change in the canting angle. These results align with a recently proposed mechanism for the enhancement of superconductivity in spin-orbit coupled rhombohedral multilayers, in which fluctuations in the spin-canting order contribute to the pairing interaction.

Magic-angle twisted trilayer graphene (MATTG) exhibits a range of strongly correlated electronic phases that spontaneously break its underlying symmetries. The microscopic nature of these phases and their residual symmetries stands as a key outstanding puzzle whose resolution promises to shed light on the origin of superconductivity in twisted materials. Here we investigate correlated phases of MATTG using scanning tunneling microscopy and identify striking signatures of interaction-driven spatial symmetry breaking. In low-strain samples, over a filling range of about 2-3 electrons or holes per moir\'e unit cell, we observe atomic-scale reconstruction of the graphene lattice that accompanies a correlated gap in the tunneling spectrum. This short-scale restructuring appears as a Kekul\'e 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 moir\'e unit cells further reveal a slow evolution of the Kekul\'e pattern, indicating that atomic-scale reconstruction coexists with translation symmetry breaking at the much longer moir\'e scale. We employ auto-correlation and Fourier analyses to extract the intrinsic periodicity of these phases and find that they are consistent with the theoretically proposed incommensurate Kekul\'e spiral order. Moreover, we find that the wavelength characterizing moir\'e-scale modulations monotonically decreases with hole doping away from half-filling of the bands and depends only weakly on the magnetic field. Our results provide essential insights into the nature of MATTG correlated phases in the presence of strain and imply that superconductivity emerges from an inter-valley coherent parent state., Comment: the main text, extended data figures, and SI

Twisted bilayer graphene (TBG) near the magic twist angle of $\sim1.1^{o}$ exhibits a rich phase diagram. However, the interplay between different phases and their dependence on twist angle is still elusive. Here, we explore the stability of various TBG phases and demonstrate that superconductivity near filling of two electrons per moir\'e unit cell alongside Fermi surface reconstructions, as well as entropy-driven high-temperature phase transitions and linear-in-T resistance occur over a range of twist angles which extends far beyond those exhibiting correlated insulating phases. In the vicinity of the magic angle, we also find a metallic phase that displays a hysteretic anomalous Hall effect and incipient Chern insulating behaviour. Such a metallic phase can be rationalized in terms of the interplay between interaction-driven deformations of TBG bands leading to Berry curvature redistribution and Fermi surface reconstruction. Our results provide an extensive perspective on the hierarchy of correlated phases in TBG as classified by their robustness against deviations from the magic angle or, equivalently, their electronic interaction requirements., Comment: main text + supplementary information

Moir\'e materials such as magic angle twisted bilayer graphene (MATBG) exhibit remarkable phenomenology, but present significant challenges for certain experimental methods, particularly scanning probes such as scanning tunneling microscopy (STM). Typical STM studies that can image tens of thousands of atomic unit cells can image roughly ten moir\'e cells, making data analysis statistically fraught. Here, we propose a method to mitigate this problem by aggregating STM conductance data from several bias voltages, and then using the unsupervised machine learning method of gaussian mixture model clustering to draw maximal insight from the resulting dataset. We apply this method, using as input coarse-grained bond variables respecting the point group symmetry, to investigate nematic ordering tendencies in MATBG for both charge neutral and hole-doped samples. For the charge-neutral dataset, the clustering reveals the surprising coexistence of multiple types of nematicity that are unrelated by symmetry, and therefore generically nondegenerate. By contrast, the clustering in the hole doped data is consistent with long range order of a single type. Beyond its value in analyzing nematicity in MATBG, our method has the potential to enhance understanding of symmetry breaking and its spatial variation in a variety of moir\'e materials.

Graphene moire superlattices have emerged as a platform hosting and abundance of correlated insulating, topological, and superconducting phases. While the origins of strong correlations and non-trivial topology are shown to be directly linked to flat moire bands, the nature and mechanism of superconductivity remain enigmatic. In particular, only alternating twisted stacking geometries of bilayer and trilayer graphene are found to exhibit robust superconductivity manifesting as zero resistance and Fraunhofer interference patterns. Here we demonstrate that magic-angle twisted tri-, quadri-, and pentalayers placed on monolayer tungsten diselenide exhibit flavour polarization and superconductivity. We also observe insulating states in the trilayer and quadrilayer arising at finite electric displacement fields, despite the presence of dispersive bands introduced by additional graphene layers. Moreover, the three multilayer geometries allow us to identify universal features in the family of graphene moire structures arising from the intricate relations between superconducting states, symmetry-breaking transitions, and van Hove singularities. Remarkably, as the number of layers increases, superconductivity emerges over a dramatically enhanced filling-factor range. In particular, in twisted pentalayers, superconductivity extends well beyond the filling of four electrons per moire unit cell, demonstrating the non-trivial role of the additional bands. Our results highlight the importance of the interplay between flat and dispersive bands in extending superconducting regions in graphene moire superlattices and open new frontiers for developing graphene-based superconductors., Comment: main text (4 figures) and supplementary information (12 figures)

Magic-angle twisted trilayer graphene (MATTG) has emerged as a novel moir\'e material that exhibits both strong electronic correlations and unconventional superconductivity. However, spectroscopic studies of its electronic properties are lacking, and the nature of superconductivity and the corresponding order parameter in this system remain elusive. Here we perform high-resolution scanning tunneling microscopy and spectroscopy of MATTG and reveal extensive regions of atomic reconstruction that favor mirror-symmetric stacking. In these regions, we observe a cascade of symmetry-breaking electronic transitions and doping-dependent band structure deformations similar to those realized in magic-angle bilayers, as expected theoretically given the commonality of flat bands. More strikingly, in a density window spanning two to three holes per moire unit cell, spectroscopic signatures of superconductivity are manifest as pronounced dips in the tunneling conductance at the Fermi level accompanied by coherence peaks that become gradually suppressed at elevated temperatures and magnetic fields. The observed evolution of the conductance with doping is consistent with a gate-tunable transition from a gapped to a nodal superconductor, which we show theoretically is compatible with a sharp transition from a Bardeen-Cooper-Schrieffer (BCS) to a Bose-Einstein condensation (BEC) superconductor with a nodal order parameter. Within this doping window, we also detect peak-dip-hump structures suggesting that superconductivity is driven by strong coupling to bosonic modes of MATTG. Our results pave the way for further understanding of superconductivity and correlated states in graphene-based moir\'e structures beyond twisted bilayers, where unconventional superconductivity and nodal pairing were reported., Comment: main text (4 figures) and methods (10 figures). References and clarifications added; typos corrected

Flat electronic bands, characteristic of magic-angle twisted bilayer graphene (TBG), host a wealth of correlated phenomena. Early theoretical considerations suggested that, at the magic angle, the Dirac velocity vanishes and the entire width of the moir\'e bands becomes extremely narrow. Yet, this scenario contradicts experimental studies that reveal a finite Dirac velocity as well as bandwidths significantly larger than predicted. Here we use spatially resolved spectroscopy in finite and zero magnetic fields to examine the electronic structure of moir\'e bands and their intricate connection to correlated phases. By following the relative shifts of Landau levels in finite fields, we detect filling-dependent band flattening, that unexpectedly starts already at ~1.3 degrees, well above the magic angle and hence nominally in the weakly correlated regime. We further show that, as the twist angle is reduced, the moir\'e bands become maximally flat at progressively lower doping levels. Surprisingly, when the twist angles reach values for which the maximal flattening occurs at approximate filling of $-2$, $+1$,$+2$,$+3$ electrons per moir\'e unit cell, the corresponding zero-field correlated phases start to emerge. Our observations are corroborated by calculations that incorporate an interplay between the Coulomb charging energy and exchange interactions; together these effects produce band flattening and hence a significant density-of-states enhancement that facilitates the observed symmetry-breaking cascade transitions. Besides emerging phases pinned to integer fillings, we also experimentally identify a series of pronounced correlation-driven band deformations and soft gaps in a wider doping range around $\pm 2$ filling where superconductivity is expected. Our results highlight the role of interaction-driven band-flattening in forming robust correlated phases in TBG., Comment: 14 pages, 4 figures, main text

Magic-angle twisted bilayer graphene (MATBG) exhibits a range of correlated phenomena that originate from strong electron-electron interactions. These interactions make the Fermi surface highly susceptible to reconstruction when $ \pm 1, \pm 2, \pm 3$ electrons occupy each moir\' e unit cell and lead to the formation of correlated insulating, superconducting and ferromagnetic phases. While some phases have been shown to carry a non-zero Chern number, the local microscopic properties and topological character of many other phases remain elusive. Here we introduce a set of novel techniques hinging on scanning tunneling microscopy (STM) to map out topological phases in MATBG that emerge in finite magnetic field. By following the evolution of the local density of states (LDOS) at the Fermi level with electrostatic doping and magnetic field, we visualize a local Landau fan diagram that enables us to directly assign Chern numbers to all observed phases. We uncover the existence of six topological phases emanating from integer fillings in finite fields and whose origin relates to a cascade of symmetry-breaking transitions driven by correlations. The spatially resolved and electron-density-tuned LDOS maps further reveal that these topological phases can form only in a small range of twist angles around the magic-angle value. Both the microscopic origin and extreme sensitivity to twist angle differentiate these topological phases from the Landau levels observed near charge neutrality. Moreover, we observe that even the charge-neutrality Landau spectrum taken at low fields is considerably modified by interactions and exhibits an unexpected splitting between zero Landau levels that can be as large as ${\sim }\,3-5$ meV. Our results show how strong electronic interactions affect the band structure of MATBG and lead to the formation of correlation-enabled topological phases.

Magic-angle twisted bilayer graphene (TBG), with rotational misalignment close to 1.1$^\circ$, features isolated flat electronic bands that host a rich phase diagram of correlated insulating, superconducting, ferromagnetic, and topological phases. The origins of the correlated insulators and superconductivity, and the interplay between them, are particularly elusive. Both states have been previously observed only for angles within $\pm0.1^\circ$ from the magic-angle value and occur in adjacent or overlapping electron density ranges; nevertheless, it is still unclear how the two states are related. Beyond the twist angle and strain, the dependence of the TBG phase diagram on the alignment and thickness of insulating hexagonal boron nitride (hBN) used to encapsulate the graphene sheets indicates the importance of the microscopic dielectric environment. Here we show that adding an insulating tungsten-diselenide (WSe$_2$) monolayer between hBN and TBG stabilizes superconductivity at twist angles much smaller than the established magic-angle value. For the smallest angle of $\theta$ = 0.79$^\circ$, we still observe clear superconducting signatures, despite the complete absence of the correlated insulating states and vanishing gaps between the dispersive and flat bands. These observations demonstrate that, even though electron correlations may be important, superconductivity in TBG can exist even when TBG exhibits metallic behaviour across the whole range of electron density. Finite-magnetic-field measurements further reveal breaking of the four-fold spin-valley symmetry in the system, consistent with large spin-orbit coupling induced in TBG via proximity to WSe$_2$. Our results highlight the importance of symmetry breaking effects in stabilizing electronic states in TBG and open new avenues for engineering quantum phases in moir\'e systems., Comment: 12 pages, 4 figures; main text

Twisted bilayer graphene with a twist angle of around 1.1{\deg} features a pair of isolated flat electronic bands and forms a strongly correlated electronic platform. Here, we use scanning tunneling microscopy to probe local properties of highly tunable twisted bilayer graphene devices and show that the flat bands strongly deform when aligned with the Fermi level. At half filling of the bands, we observe the development of gaps originating from correlated insulating states. Near charge neutrality, we find a previously unidentified correlated regime featuring a substantially enhanced flat band splitting that we describe within a microscopic model predicting a strong tendency towards nematic ordering. Our results provide insights into symmetry breaking correlation effects and highlight the importance of electronic interactions for all filling factors in twisted bilayer graphene., Comment: Main text 9 pages, 4 figures; Supplementary Information 25 pages