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The recent discovery of superconductivity and magnetism in trilayer rhombohedral graphene (RG) establishes an ideal, untwisted platform to study strong correlation electronic phenomena. However, the correlated effects in multilayer RG have received limited attention, and, particularly, the evolution of the correlations with increasing layer number remains an unresolved question. Here, we show the observation of layer-dependent electronic structures and correlations in RG multilayers from 3 to 9 layers by using scanning tunneling microscopy and spectroscopy. We explicitly determine layer-enhanced low-energy flat bands and interlayer coupling strength. The former directly demonstrates the further flattening of low-energy bands in thicker RG, and the later indicates the presence of varying interlayer interactions in RG multilayers. Moreover, we find significant splitting of the flat bands, ranging from ~50-80 meV, under liquid nitrogen temperature when they are partially filled, indicating the emergence of interaction-induced strongly correlated states. Particularly, the strength of the correlated states is notably enhanced in thicker RG and reaches its maximum in the six-layer, validating directly theoretical predictions and establishing abundant new candidates for strongly correlated systems. Our results provide valuable insights into the layer dependence of the electronic properties in RG, paving the way for investigating robust and highly accessible correlated phases in simpler systems., Comment: 21 pages, 4 figures

Metal chalcogenide is a promising material for studying novel underlying physical phenomena and nanoelectronics applications. Here, we systematically investigate the crystal structure and electronic properties of the AlSe surface alloy on Al (111) using scanning tunneling microscopy, angle-resolved photoelectron spectrometer, and first-principle calculations. We reveal that the AlSe surface alloy possesses a hexagonal closed-packed structure. The AlSe surface alloy comprises two atomic sublayers (Se sublayer and Al sublayer) with 1.16 A along the z direction. The dispersion shows two hole-like bands for AlSe surface alloy located at about -2.2 eV, far below the Fermi level, which is sharply different from other metal chalcogenide and binary alloys. These two bands mainly derive from the in-plane orbital of AlSe (px and py). These results provide implications for related Al-chalcogen interface. Meanwhile, AlSe alloy have an advantage of large-scale atomic flatness and a wide band gap near the Fermi level in serving as an interface for two-dimensional materials., Comment: 15 pages, 5 figures

Nickel ditelluride (NiTe2), a new discovered type-II Dirac semimetal whose Dirac node lies close to its Fermi level, is expected to exhibit exotic phenomena including Lifshitz transition and superconductivity. As we know, defects are inevitable for transition metal dichalcogenides and have significant impacts on the optical and electronic properties. However, the systematic study of defects in NiTe2 is still lack. Here, by using high-resolution scanning tunneling microscopy combined with first-principles calculations, the point defects including the vacancy, intercalation and antisite defects in NiTe2 are systematically investigated. We identified five main types native defects and revealed that the growth condition could affect the type of native defects. By controlling the ratio of ingredient during synthesis, the types of point defects are expected to be manipulated, especially antisite defects. Additionally, we find native defects could slightly dope the topological surface states. Our results provide a facile way to manipulate defects for future optimizing the electronic properties of NiTe2 and other related materials., Comment: 17 pages, 4 figures, 1 table

With considering the great success of scanning tunnelling microscopy (STM) studies of graphene in the past few years, it is quite surprising to notice that there is still a fundamental contradiction about the reported tunnelling spectra of quasi-free-standing graphene monolayer. Many groups observed V-shape spectra with linearly vanishing density-of-state (DOS) at the Dirac point, whereas, the others reported spectra with a gap of 60 meV pinned to the Fermi level in the quasi-free-standing graphene monolayer. Here we systematically studied the two contradicted tunnelling spectra of the quasi-free-standing graphene monolayer on several different substrates and provided a consistent interpretation about the result. The gap in the spectra arises from the out-of-plane phonons in graphene, which mix the Dirac electrons at the Brillouin zone corners with the nearly free-electron states at the zone center. Our experiment indicated that interactions with substrates could effectively suppress effects of the out-of-plane phonons in graphene and enable us to detect only the DOS of the Dirac electrons in the spectra. We also show that it is possible to switch on and off the out-of-plane phonons of graphene at the nanoscale, i.e., the tunnelling spectra show switching between the two distinct features, through voltage pulses applied to the STM tip., Comment: 4 Figures

Nanoscale twisted bilayer graphene (TBG) is quite instable and will change its structure to Bernal (or AB-stacking) bilayer with a much lower energy. Therefore, the lack of nanoscale TBG makes its electronic properties not accessible in experiment up to now. In this work, a special confined TBG is obtained in the overlaid area of two continuous misoriented graphene sheets. The width of the confined region of the TBG changes gradually from about 22 nm to 0 nm. By using scanning tunnelling microscopy, we studied carefully the structure and the electronic properties of the nanoscale TBG. Our results indicate that the low-energy electronic properties, including twist-induced van Hove singularities (VHSs) and spatial modulation of local density-of-state, are strongly affected by the translational symmetry breaking of the nanoscale TBG. Whereas, the electronic properties above the energy of the VHSs are almost not influenced by the quantum confinement even when the width of the TBG is reduced to only a single moire spot., Comment: 4 Figures

When electrons are confined in a two dimensional (2D) system, typical quantum mechanical phenomena such as Landau quantization can be detected. Graphene systems, including the single atomic layer and few-layer stacked crystals, are ideal 2D materials for studying a variety of quantum mechanical problems. In this article, we review the experimental progress in the unusual Landau quantized behaviors of Dirac fermions in monolayer and multilayer graphene by using scanning tunneling microscopy(STM) and scanning tunneling spectroscopy(STS). Through STS measurement of the strong magnetic fields, distinct Landau-level spectra and rich level splitting phenomena are observed in different graphene layers. These unique properties provide an effective method for identifying the number of layers, as well as the stacking orders, and investigating the fundamentally physical phenomena of graphene. Moreover, in the presence of a strain and charged defects, the Landau quantization of graphene can be significantly modified, leading to unusual spectroscopic and electronic properties.

The interlayer gallery between two adjacent sheets of van der Waals materials is expected to modify properties of atoms and molecules confined at the atomic interfaces. Here, we directly image individual hydrogen atom intercalated between two graphene sheets and investigate its dynamics by scanning tunnelling microscope (STM). The intercalated hydrogen atom is found to be remarkably different from atomic hydrogen chemisorbed on external surface of graphene. Our STM measurements, complemented by first-principles calculations, show that the hydrogen atom intercalated between two graphene sheets has dramatically reduced potential barriers for elementary migration steps. Especially, the confined atomic hydrogen dissociation energy from graphene is reduced to 0.34 eV, which is only about a third of a hydrogen atom chemisorbed on graphene. This offers a unique platform for direct imaging of the atomic dynamics of confined atoms. Our results suggest that the atomic interfaces of van der Waals materials may provide a confined environment to tune the interfacial chemical reactions., Comment: 5 figures

A variety of new and interesting correlated states have been predicted in graphene monolayer doped to Van Hove singularities (VHSs) of its density-of-state (DOS). However, tuning the Fermi energy to reach a VHS of graphene by either gating or chemical doping is prohibitively difficult, owning to their large energy distance (3 eV). Therefore, these correlated states, which arise from effects of strong electron-electron interactions at the VHSs, have remained experimentally elusive. Here, we report experimental evidences of electron-electron interactions around the VHSs of a twisted bilayer graphene (TBG) through scanning tunneling microscopy measurements. By introducing a small twisted angle between two adjacent graphene sheets, we are able to generate low-energy VHSs arbitrarily approaching the Fermi energy. The split of the VHSs are observed and the symmetry breaking of electronic states around the VHSs are directly visualized. These results experimentally demonstrate the important effects of electron-electron interactions on electronic properties around the VHSs of the TBG, therefore providing motivation for further theoretical and experimental studies in graphene systems with considering many-body interactions., Comment: 4 Figures in main text

Trilayer graphene (TLG) exhibits rich novel electronic properties and extraordinary quantum Hall phenomena owning to enhanced electronic interactions and tunable chirality of its quasiparticles. Here, we report direct observation of chirality transition of quasiparticles at stacking solitons of TLG via spatial-resolved Landau level spectroscopy. The one-dimensional stacking solitons with width of the order of 10 nm separate adjacent Bernal-stacked TLG and rhombohedral-stacked TLG. By using high field tunneling spectra of scanning tunneling microscopy, we measured Landau quantization in both the Bernal-stacked TLG and the rhombohedral-stacked TLG and, importantly, we observed evolution of quasiparticles between the chiral degree l = 1&2 and l = 3 across the stacking domain wall solitons. Our experiment indicates that such a chirality transition occurs smoothly, accompanying the transition of the stacking orders of TLG, around the domain wall solitons. This result demonstrates the important and hitherto neglected relationship between the crystallographic stacking order and the chirality of quasiparticles in graphene systems., Comment: 4 Figures

The pristine graphene is strongly diamagnetic. However, graphene with single carbon atom defects could exhibit paramagnetism with local magnetic moments ~ 1.5 per vacancy1-6. Theoretically, both the electrons and electrons of graphene contribute to the magnetic moment of the defects, and the pi magnetism is characterizing of two spin-split DOS (density-of-states) peaks close to the Dirac point1,6. Since its prediction, many experiments attempt to study this pi magnetism in graphene, whereas, only a notable resonance peak has been observed around the atomic defects6-9, leaving the pi magnetism experimentally so elusive. Here, we report direct experimental evidence of the pi magnetism by using scanning tunnelling microscope. We demonstrate that the localized state of the atomic defects is split into two DOS peaks with energy separations of several tens meV and the two spin-polarized states degenerate into a profound peak at positions with distance of ~ 1 nm away from the monovacancy. Strong magnetic fields further increase the energy separations of the two spin-polarized peaks and lead to a Zeeman-like splitting. The effective g-factors geff around the atomic defect is measured to be about 40. Such a giant enhancement of the g-factor is attributed to the strong spin polarization of electron density and large electron-electron interactions near the atomic vacancy., Comment: 4 Figures in main text

Graphene nanoribbons (GNRs) are one-dimensional (1D) structures that exhibit a rich variety of electronic properties1-17. Therefore, they are predicted to be the building blocks in next-generation nanoelectronic devices. Theoretically, it has been demonstrated that armchair GNRs can be divided into three families, i.e., Na = 3p, Na = 3p + 1, and Na = 3p + 2 (here Na is the number of dimer lines across the ribbon width and p is an integer), according to their electronic structures, and the energy gaps for the three families are quite different even with the same p1,3-6. However, a systematic experimental verification of this fundamental prediction is still lacking, owing to very limited atomic-level control of the width of the armchair GNRs investigated7,9,10,13,17. Here, we studied electronic structures of the armchair GNRs with atomically well-defined widths ranging from Na = 6 to Na = 26 by using scanning tunnelling microscope (STM). Our result demonstrated explicitly that all the studied armchair GNRs exhibit semiconducting gaps due to quantum confinement and, more importantly, the observed gaps as a function of Na are well grouped into the three categories, as predicted by density-functional theory calculations3. Such a result indicated that we can tune the electronic properties of the armchair GNRs dramatically by simply adding or cutting one carbon dimer line along the ribbon width., Comment: 5 figures

In strained graphene, lattice deformation can create pseudo-magnetic fields and result in zero-field Landau level-like quantization. In the presence of an external magnetic field, valley-polarized Landau levels are predicted to be observed because the pseudo-magnetic fields are of opposite directions in the K and K' valleys of graphene. Here, we present experimental spectroscopic measurements by scanning tunneling microscopy of strained graphene on Rh foil. We direct observed valley splitting of the Landau level induced by the coexistence of the pseudo-magnetic fields and external magnetic fields. The observed result paves the way to exploit novel electronic properties in graphene through the combination of the pseudo-magnetic fields and the external magnetic fields., Comment: 3 Figures in main text and 3 figures in Supplementary Materials

The wavefunction of massless Dirac fermions is a two-component spinor. In graphene, a one-atom-thick film showing two-dimensional Dirac-like electronic excitations, the two-component representation reflects the amplitude of the electron wavefunction on the A and B sublattices. This unique property provides unprecedented opportunities to image the two components of massless Dirac fermions spatially. Here we report atomic resolution imaging of the two-component Dirac-Landau levels in a gapped graphene monolayer by scanning tunnelling microscopy and spectroscopy. A gap of about 20 meV, driven by inversion symmetry breaking by the substrate potential, is observed in the graphene on both SiC and graphite substrates. Such a gap splits the n = 0 Landau level (LL) into two levels, 0+ and 0-. We demonstrate that the amplitude of the wavefunction of the 0- LL is mainly at the A sites and that of the 0+ LL is mainly at the B sites of graphene, characterizing the internal structure of the spinor of the n = 0 LL. This provides direct evidence of the two-component nature of massless Dirac fermions., Comment: 4 Figures in main text and 4 Figures in SI

We use the tip of the scanning tunneling microscope (STM) to manipulate single weakly bound nanometer-sized sheets on the the highly oriented pyrolytic graphite (HOPG) surface through artifically increasing the tip and sample interaction in humid environment. By this means it is possible to tear apart a graphite sheet againt a step and fold this part onto the HOPG surface and thus generate the gaphene superlattices with hexagonal symmetry. The tip and sample surface interactions, including the van der Waals force, eletrostatic force and capillary attraction force originating from the Laplace pressure due to the formation of a highly curved fluid meniscus connecting the tip and sample, are discussed in details to understand the fromation mechnism of graphen superlattice induced by the STM tip. Especially, the capillary force is the key role in manipulating the graphite surface sheet in the hunmidity condition. Our approach may provides a simple and feasible route to prepare the controllable superlattices and graphene nanoribbons but also replenish and find down the theory of generation of graphene superlattice on HOPG surface by the tip., Comment: 17 pages, 5 figures

Despite the structures and properties of tilt grain boundaries of graphite surface and graphene have been extensively studied, their effect on the structures and electronic spectra of graphene layers has not been fully addressed. Here we study effects of one-dimensional tilt grain boundaries on structures and electronic spectra of graphene multilayers by scanning tunneling microscopy and spectroscopy. A tilt grain boundary of a top graphene sheet in graphene multilayers leads to a twist between consecutive layers and generates superstructures (Moir\'e patterns) on one side of the boundary. Our results demonstrate that the twisting changes the electronic spectra of Bernal graphene bilayer and graphene trilayers dramatically. We also study quantum-confined twisted graphene bilayer generated between two adjacent tilt grain boundaries and find that the band structure of such a system is still valid even when the number of superstructures is reduced to two in one direction. It implies that the electronic structure of this system is driven by the physics of a single Moir\'e spot., Comment: 4 figures in main text and 8 figures in SI