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Many intriguing quantum states of matter, such as unconventional superconductivity, magnetic phases and fractional quantum Hall physics, emergent from the spatially-correlated localized electrons in the flat band of solid materials. By using scanning tunneling microscopy and spectroscopy (STM/STS), we report the real-space investigation of correlated electrons in the flat band of superlattice 4Hb-TaSexS2-x. In contrast with the pristine 4Hb-TaS2, the selenium (Se) substitutions significantly affect the interfacial transfer of correlated electrons between the CDW states of 1T- and 1H-TaS2 layers, and contribute a real-space fractional electron-filling configurations with the distributed electron-filled and -void SoD clusters of 1T-layer. The site-specific STS spectra directly reveal their respective prominent spectra weight above EF and symmetric Mott-like spectra. In addition, the spatial distributions of these electron-filled SoDs in the 1T-layer of 4Hb-TaSe0.7S1.3 demonstrate different local short-range patterning, clearly indicating the complex neighboring interactions among the localized electrons in the flat band of 1T-layer. Our results not only provide an in-depth insight of correlated electrons in the flat CDW band, and provide a simple platform to manipulate the electron-correlation-related quantum states., Comment: 18 pages, 4 figures

Fe5GeTe2 single crystals can be divided into nonquenched (NQ) and quench-cooled (QC) phases with different magnetic properties. A comprehensive understanding of the magnetic property variations in the NQ and QC phases is imperative for guiding Fe5GeTe2 towards spintronics applications; however, it remains elusive. Here, we report a real-space study on the structural and magnetic properties of these two magnetic phases using cryogenic magnetic force microscopy and scanning tunneling microscopy. The thermal history introduces disorder and order to the Fe(1) sites, resulting in the NQ and QC phases exhibiting global and broken inversion symmetry, respectively. The observed magnetic domain transitions (branching to labyrinthine) in the spin reorientation process and the distinct 3D spin textures stabilized by magnetic dipolar interaction observed in field-dependent studies allow the NQ phase to exhibit a more resilient global magnetic state. In contrast, the QC phase exhibits enhanced magnetic anisotropy, resulting in a higher TC. Meanwhile, the Dzyaloshinskii-Moriya interaction (DMI) introduced by the broken inversion symmetry causes the QC phase to exhibit a localized magnetic state: no domain transformation occurs during spin reorientation, and irregular domain states are observed in field-related studies. Our work provides an important reference for understanding the complex magnetic properties in Fe5GeTe2., Comment: 18 pages,4 figures

The complex correlated charge density wave (CDW) phases of 1T-TaS2 have attracted great attention due to their emergent quantum states, such as intricate CDW phase, Mott-Hubbard state, superconductivity and quantum spin liquid. The delicate interplay among the complex intra-/inter-layer electron-electron and electron-lattice interactions is the fundamental prerequisite of these exotic quantum states. Here, we report a real-space titration-like investigation of correlated CDW state in 1T-TaS2 upon hole-doping via low-temperature scanning tunneling microscopy (LT-STM). The gradual increased hole-doping results in the sequential emergence of electron voids, phase domains, stacking disordering and mixed phase/chiral domains attributed to the reduced electron correlations. The achiral intermediate ring-like clusters and nematic CDW states emerge at the intralayer chiral domain wall and interlayer heterochiral stacking regions via the chiral-overlapping configurations. The local reversible CDW manipulation is further realized by the non-equilibrium transient charge-injections of STM field-emission spectra. Our results provide an in-depth insight of this intricate correlated CDW state, and pave a way to realize exotic quantum states via the accurate tuning of interior interactions in correlated materials.

Kagome-lattice materials possess attractive properties for quantum computing applications, but their synthesis remains challenging. Herein, we show surface kagome electronic states (SKESs) on a Sn-terminated triangular Co3Sn2S2 surface, which are imprinted by vertical p-d electronic hybridization between the surface Sn (subsurface S) atoms and the buried Co kagome lattice network in the Co3Sn layer under the surface. Owing to the subsequent lateral hybridization of the Sn and S atoms in a corner-sharing manner, the kagome symmetry and topological electronic properties of the Co3Sn layer is proximate to the Sn surface. The SKESs and both hybridizations were verified via qPlus non-contact atomic force microscopy (nc-AFM) and density functional theory calculations. The construction of SKESs with tunable properties can be achieved by the atomic substitution of surface Sn (subsurface S) with other group III-V elements (Se or Te), which was demonstrated theoretically. This work exhibits the powerful capacity of nc-AFM in characterizing localized topological states and reveals the strategy for synthesis of large-area transition-metal-based kagome lattice materials using conventional surface deposition techniques.

Recently, 2D Cr5Te8 has been successfully synthesized experimentally and has attracted widespread research interest due to its intriguing magnetic properties, such as hard magnetism with strong perpendicular anisotropy. However, exploring new methods for growing ultrathin 2D Cr5Te8 with a larger scale and their controllable synthesis remain challenging. Herein, the synthesis of ultrathin 2D ferromagnetic Cr5Te8 nanosheets by chemical vapor deposition (CVD) using GaTe as growth source is reported, whose size is up to ~160 {\mu}m and the thickness is lower to only 5 nm. The GaTe promotes the concentration of effective Te atoms to facilitate the direction of the synthesis reaction, enabling the rapid lateral growth rate. As a result, the synthesis of ultrathin, large-scale 2D ferromagnetic Cr5Te8 was achieved. By precisely adjusting the growth temperature and the source-substrate distance (Dss), the lateral size of the Cr5Te8 nanosheets can be tuned from a few to ~164 {\mu}m. Furthermore, magnetic property measurement system (MPMS) suggested that Cr5Te8 nanosheets possess intense out-of-plane ferromagnetism and the Curie temperature exhibits a monotonic increase from 163 to 175 K as the Cr5Te8 thickness. This work not only paves a way for the controllable growth of ultrathin, large-scale 2D ferromagnetic crystalline, but also provides a new platform for the spintronics and the practical application of magnetic memory devices., Comment: arXiv admin note: substantial text overlap with arXiv:2302.11422

As a typical 2D magnetic material with self-intercalated structure, Cr5Te8 exhibits many fascinating magnetic properties. Although the ferromagnetism of 2D Cr5Te8 has been reported, the study of its magnetic domain is still blank. Herein, we successfully fabricated 2D Cr5Te8 nanosheets with controlled thickness and lateral size by chemical vapor deposition (CVD). Then magnetic property measurement system suggested Cr5Te8 nanosheets possessing intense out-of-plane ferromagnetism with the Curie temperature of 179 K. Most importantly, we found magnetic bubbles and thickness-dependent maze-like magnetic domains by cryogenic magnetic force microscopy (MFM) for the first time. The domain width of the maze-like magnetic domains increases rapidly with decreasing sample thickness, while domain contrast decreases. This indicates dipolar interaction is the dominant role over exchange interaction and magnetic anisotropy. Our work not only paves a way for the controllable growth of 2D magnetic materials, but also suggests new directions for controlling magnetic phases and systematically adjusting domain properties.

Polymorphic structures of transition-metal dichalcogenides (TMDs) host exotic electronic states, like charge density wave and superconductivity. However, the number of these structures is limited by crystal symmetries, which poses a challenge to achieve tailored lattices and properties both theoretically and experimentally. Here, we report a coloring-triangle (CT) latticed MoTe2 monolayer, termed CT-MoTe2, constructed by controllably introducing uniform and ordered mirror-twin-boundaries into a pristine monolayer in molecular beam epitaxy. Low-temperature scanning tunneling microscopy and spectroscopy (STM/STS) together with theoretical calculations reveal that the monolayer has an electronic Janus lattice, i.e., an energy-dependent atomic-lattice and a pseudo-Te sublattice, and shares the identical geometry with the Mo5Te8 layer. Dirac-like and flat electronic bands inherently existing in the CT lattice are identified by two broad and two prominent peaks in STS spectra, respectively, and verified with density-functional-theory calculations. Two types of intrinsic domain boundaries were observed, in one of which the electronic-Janus-lattice feature maintains, implying potential applications as an energy-tunable electron-tunneling barrier in future functional devices.

Correlated two-dimensional (2D) layers, like 1T-phases of TaS2, TaSe2 and NbSe2, exhibit rich tunability through varying interlayer couplings, which promotes the understanding of electron-correlation in the 2D limit. However, the coupling mechanism is, so far, poorly understood and was tentatively ascribed to interactions among the d_(z^2 ) orbitals of Ta or Nb atoms. Here, we theoretically show that the interlayer hybridization and localization strength of interfacial Se pz orbitals, rather than Nb d_(z^2 ) orbitals, govern the variation of electron-correlated properties upon interlayer sliding or twisting in correlated magnetic 1T-NbSe2 bilayers. Each of the both layers is in a star-of-David (SOD) charge-density-wave phase. Geometric and electronic structures, and magnetic properties of 28 different stacking configurations were examined and analyzed using density-functional-theory calculations. We found that the SOD contains a localized region (Reg-L), in which interlayer Se pz hybridization plays a paramount role in varying the energy levels of the two Hubbard bands. These variations lead to three electronic transitions among four insulating states, which demonstrated the effectiveness of interlayer interactions to modulate correlated magnetic properties in a prototypical correlated magnetic insulator., Comment: 5 figures

Quantum materials with tunable correlated and/or topological electronic states, such as the electronic Kagome lattice, provide an ideal platform to study the exotic quantum properties. However, the real-space investigations on the correlated electronic Kagome lattice have been rarely reported. Herein, we report on the electronic Kagome lattice emerging in the correlated charge-density-wave (CDW) state of 1T-TaS$_2$ at ~200 K via variable-temperature scanning tunneling microscopy (VT-STM). This emergent Kagome lattice can be considered a fractional electron-filling superstructure with reduced translational and rotational symmetries, confirmed by STM measurements and density functional theory simulations. The characteristic band structure and density of states of this electronic Kagome lattice are further explored based on theoretical calculations. Our results demonstrate a self-organized electronic Kagome lattice from the correlated CDW state via the effective tuning parameter of temperature and provide a platform to directly explore the interplay of correlated electrons and topological physics., Comment: 20 pages, 4figures

Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline substrates. However, in principle, this success in monolayer epitaxy seems extremely difficult to be replicated to bi- or few-layer growth, as the full coverage of the first layer was believed to terminate the reactivity of those adopting catalytic metal surfaces. Here, we report an exceptional layer-by-layer chemical vapour deposition (CVD) growth of large size bi-layer graphene single-crystals, enabled by self-transmitting catalytic activity from platinum (Pt) surfaces to the outermost graphene layers. In-situ growth and real-time surveillance experiments, under well-controlled environments, unambiguously verify that the growth does follow the layer-by-layer mode on open surfaces of MLG/Pt(111). First-principles calculations indicate that the transmittal of catalytic activity is allowed by an appreciable electronic hybridisation between graphene overlayers and Pt surfaces, enabling catalytic dissociation of hydrocarbons and subsequently direct graphitisation of their radicals on the outermost sp2 carbon surface. This self-transmitting catalytic activity is also proven to be robust for tube-furnace CVD in fabricating single-crystalline graphene bi-, tri- and tetra-layers, as well as h-BN few-layers. Our findings offer an exceptional strategy for potential controllable, layer-by-layer and wafer-scale growth of vertically stacked few-layered 2D single crystals., Comment: 5 figures and 9 extended figures

In this work, a novel method to grow high-quality and large bilayer graphene (BLG) directly on various dielectric substrates was demonstrated. Large area single-crystal monolayer graphene was applied as a seeding layer to facilitate the homo-epitaxial synthesis of single crystal BLG directly on insulating substrates. The Cu nano-powders (Cu NP) with nanostructure and high surface-area were used as the remote catalysis to provide long-lasting catalytic activity during the graphene growth. The TEM results confirmed the single-crystalline nature of the BLG domains, which validates the superiority of the homo-epitaxial growth technique. The as-grown BLG show comparable quality with the CVD-grown BLG on metal surface. Field-effect transistors directly fabricated on the as-grown BLG/SiO$ _2 $/Si showed a room temperature carrier mobility as high as 2297 cm $ ^2 $ V$ ^{-1}$ s $^{-1} $.

Tailoring the interlayer twist angle of bilayer graphene (BLG) has a significant influence on its electronic properties, including superconductivity, topological transitions, ferromagnetic states and correlated insulating states. These exotic electronic properties are sensitively dependent on the work functions of bilayer graphene samples. Here, the twisted angle-dependent work functions of CVD-grown twisted bilayer graphene (tBLG) are detailed investigated by Kelvin Probe Force Microscopy (KPFM) in combination with Raman spectra. The thickness-dependent surface potentials of Bernal-stacked multilayer graphene were measured. The AB-BLG and tBLG are directly determined by KPFM due to their twist angle-specific surface potentials. The detailed relationship of twist angles and surface potentials are further obtained by the in-situ combination investigation of KPFM and Raman spectra measurements. The thermal stability of tBLG was further explored through controlled annealing process. Our work provides the twisted angle-dependent surface potentials of tBLG and lays the foundation for further exploring their twist-angle-dependent novel electronic properties.

Magnetic topological insulators (MTIs) have received a lot of attention due to the existence of various quantum phenomena such as quantum anomalous Hall effect (QAHE) and topological magnetoelectric effect, etc. The intrinsic superlattice-like layered MTIs, MnBi2Te4/(Bi2Te3)n, have been extensively investigated mainly through the transport measurements, while the direct investigation of their superlattice-sensitive magnetic behaviors is relatively rare. Here, we report a microscopic real-space investigation of magnetic phase behaviors in MnBi4Te7 using cryogenic magnetic force microscopy (MFM). The intrinsic robust A-type antiferromagnetic (AFM), and emerged surface spin-flop (SSF), canted AFM (CAFM), ferromagnetic (FM)+CAFM, forced FM phases are sequentially visualized via the increased external magnetic field, in agreement with the metamagnetic behavior in the M-H curve. The temperature-dependent magnetic phase evolution behaviors are further investigated to obtain the complete H-T phase diagram of MnBi4Te7. The tentative local phase manipulation via the stray field of the magnetic tip is demonstrated by transforming the AFM to FM phase in its surface layers of MnBi4Te7. Our study the not only provide key real-space ingredients for understanding their complicated magnetic, electronic, and topological properties of these intrinsic MTIs, but also suggest new directions for manipulating spin textures and locally controlling their exotic properties.

Electronic properties of super-atomic crystals have not been sufficiently explored due to the versatility of their building units; moreover, their inter-unit couplings are even poorly understood. Here, we present a joint experiment-theory investigation of a rational-designed layered super-atomic crystal of Au6Te12Se8 cubes, stacked by non-covalent inter-cube quasi-bonds. We found a sequential-emerged anisotropic triple-cube charge-density-wave (tc-CDW) and polarized metallic states below 120 K, as revealed via scanning tunneling microscopy/spectroscopy, angle-resolved photoemission spectroscopy, transport measurement, Raman spectra, and density functional theory. The polarized states are locked in an anti-parallel configuration, which is required for maintaining the inversion symmetry of the center-cube in the tc-CDW. The anti-polar metallic states are thus interweaved by the charge-density-wave and the polarized metallic states, and primarily ascribed to electronic effects via theoretical calculations. This work not only demonstrates a microscopic picture of the interweaved CDW and polarized charge orders in the super-atomic crystal of ATS, but also sheds light on expanding the existing category of quantum materials to non-covalent solids., Comment: 15 pages, 4 figures, to be appeared in Physical Review X

Transition-metal chalcogenides (TMCs) materials have attracted increasing interest both for fundamental research and industrial applications. Among all these materials, two-dimensional (2D) compounds with honeycomb-like structure possess exotic electronic structures. Here, we report a systematic study of TMC monolayer AgTe fabricated by direct depositing Te on the surface of Ag(111) and annealing. Few intrinsic defects are observed and studied by scanning tunneling microscopy, indicating that there are two kinds of AgTe domains and they can form gliding twin-boundary. Then, the monolayer AgTe can serve as the template for the following growth of Te film. Meanwhile, some Te atoms are observed in the form of chains on the top of the bottom Te film. Our findings in this work might provide insightful guide for the epitaxial growth of 2D materials for study of novel physical properties and for future quantum devices., Comment: 16 pages, 5 figures

Nanocontact properties of two-dimensional (2D) materials are closely dependent on their unique nanomechanical systems, such as the number of atomic layers and the supporting substrate. Here, we report a direct observation of toplayer-dependent crystallographic orientation imaging of 2D materials with the transverse shear microscopy (TSM). Three typical nanomechanical systems, MoS2 on the amorphous SiO2/Si, graphene on the amorphous SiO2/Si, and MoS2 on the crystallized Al2O3, have been investigated in detail. This experimental observation reveals that puckering behaviour mainly occurs on the top layer of 2D materials, which is attributed to its direct contact adhesion with the AFM tip. Furthermore, the result of crystallographic orientation imaging of MoS2/SiO2/Si and MoS2/Al2O3 indicated that the underlying crystalline substrates almost do not contribute to the puckering effect of 2D materials. Our work directly revealed the top layer dependent puckering properties of 2D material, and demonstrate the general applications of TSM in the bilayer 2D systems.

The interlayer bonding in two dimensional materials is particularly important because it is not only related to their physical and chemical stability but also affects their mechanical, thermal, electronic, optical, and other properties. To address this issue, we report the direct characterization of the interlayer bonding in 2D SnSe using contact-resonance atomic force microscopy in this study. Site specific CR spectroscopy and CR force spectroscopy measurements are performed on both SnSe and its supporting SiO2 substrate comparatively. Based on the cantilever and contact mechanic models, the contact stiffness and vertical Young's modulus are evaluated in comparison with SiO2 as a reference material. The interlayer bonding of SnSe is further analyzed in combination with the semi-analytical model and density functional theory calculations. The direct characterization of interlayer interactions using this nondestructive methodology of CR AFM would facilitate a better understanding of the physical and chemical properties of 2D layered materials, specifically for interlayer intercalation and vertical heterostructures., Comment: 22 pages, 6 figures

At least four two- or quasi-one- dimensional allotropes and a mixture of them were theoretically predicted or experimentally observed for low-dimensional Te, namely the {\alpha}, \b{eta}, {\gamma}, {\delta} and chiral-{\alpha}+{\delta} phases. Among them the {\gamma} and {\alpha} phases were found the most stable phases for monolayer and thicker layers, respectively. Here, we found two novel low-dimensional phases, namely the {\epsilon} and {\zeta} phases. The {\zeta} phase is over 29 meV/Te more stable than and the {\epsilon} phase shows comparable stability with the most stable monolayer {\gamma} phase. The energetic difference between the {\zeta} and {\alpha} phases reduces with respect to the increased layer thickness and vanishes at the four-layer (12-sublayer) thickness, while this thickness increases under change doping. Both {\epsilon} and {\zeta} phases are metallic chains and layers, respectively. The {\zeta} phase, with very strong interlayer coupling, shows quantum well states in its layer-dependent bandstructures. These results provide significantly insight into the understanding of polytypism in Te few-layers and may boost tremendous studies on properties of various few-layer phases., Comment: 3 figures with 9 SI figures and 3 SI tables

Recently, a covalent-like quasi-bonding was unveiled for the inter-chain interaction in a promising semiconductor, few-layer Tellurium. Such quasi-bond offers comparable bond lengths and strengths with those of a typical Te-Te covalent bond, which may lead to much easier transformations between the quasi-bonds and the covalent bonds. Here, we show a few structural phase-transitions among four Te allotropes in few-layer Te under charge doping. In particular, the semiconducting {\alpha}-phase can transform into a smaller-bandgap {\beta}-phase, even-smaller-bandgap {\gamma}-phase and then metallic {\delta}-phase in a Te bilayer. In a tri-layer, a metallic chiral {\alpha}+{\delta} phase is more stable under initial electron doping, leading to the appearance of chirality. Variations of electronic structures aside, these transitions are accompanied by the emergence or elimination of inversion centers ({\alpha}-{\beta}, {\alpha}-{\gamma}, {\alpha}-{\alpha}+{\delta}), structural anisotropy ({\alpha}-{\gamma}, {\gamma}-{\delta}) and chirality ({\alpha}-{\alpha}+{\delta}), which could result in substantial changes in optical and other properties. In light of this, this work opens the possibility toward building mono-elemental electronic and optoelectronic heterostructures or devices. It also offers a platform for studying relations between charge doping and electric/optical properties.

Monolayer lateral heterostructure of graphene and hexagonal boron nitride (h-BNC) has attracted a growing attention mainly due to its tunable band-gap character and unique physical properties at interface. Hereby, we reported the first-time synthesis of a nearly freestanding h-BNC hybrid on a weakly coupled substrate of Ir (111), where graphene and h-BN possessing different surface heights and corrugations formed a perfect monolayer hybrid. With the aid of scanning tunneling microscopy/spectroscopy (STM/STS), we demonstrated that h-BN can patch alongside the boundary of pre-deposited graphene domains and vice versa to form a seamless monolayer hybrid, with the realization of predominant zigzag type chiral boundaries at the interface. Density-functional theory calculations and STM/STS measurements aided us to reveal that this interface between graphene and h-BN were atomically sharp in aspects of the chemical bonding as well as the local electronic property from both theoretical and experimental points of view., Comment: 17 pages, 5 figures