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Dimensional modifications play a crucial role in various applications, especially in the context of device miniaturization, giving rise to novel quantum phenomena. The many-body dynamics induced by dimensional modifications, including electron-electron, electron-phonon, electron-magnon and electron-plasmon coupling, are known to significantly affect the atomic and electronic properties of the materials. By reducing the dimensionality of orthorhombic CoSe2 and forming heterostructure with bilayer graphene using molecular beam epitaxy, we unveil the emergence of two types of phase transitions through angle-resolved photoemission spectroscopy and scanning tunneling microscopy measurements. We disclose that the 2 × 1 superstructure is associated with charge density wave induced by Fermi surface nesting, characterized by a transition temperature of 340 K. Additionally, another phase transition at temperature of 160 K based on temperature dependent gap evolution are observed with renormalized electronic structure induced by electron-boson coupling. These discoveries of the electronic and atomic modifications, influenced by electron-electron and electron-boson interactions, underscore that many-body physics play significant roles in understanding low-dimensional properties of non-van der Waals Co-chalcogenides and related heterostructures.

The family of transition-metal dipnictides has been of theoretical and experimental interest because this family hosts topological states and extremely large magnetoresistance (MR). Recently,TaAs2, a member of this family, has been predicted to support a topological crystalline insulating state. Here, by using high-resolution angle-resolved photoemission spectroscopy (ARPES), we reveal both closed and open pockets in the metallic Fermi surface (FS) and linearly dispersive bands on the (2‾01) surface, along with the presence of extreme MR observed from magneto-transport measurements. A comparison of the ARPES results with first-principles computations shows that the linearly dispersive bands on the measured surface ofTaAs2are trivial bulk bands. The absence of symmetry-protected surface state on the (2‾01) surface indicates its topologically dark nature. The presence of open FS features suggests that the open-orbit fermiology could contribute to the extremely large MR ofTaAs2.

Tunability of interfacial effects between two-dimensional (2D) crystals is crucial not only for understanding the intrinsic properties of each system, but also for designing electronic devices based on ultra-thin heterostructures. A prerequisite of such heterostructure engineering is the availability of 2D crystals with different degrees of interfacial interactions. In this work, we report a controlled epitaxial growth of monolayer TaSe2 with different structural phases, 1H and 1 T, on a bilayer graphene (BLG) substrate using molecular beam epitaxy, and its impact on the electronic properties of the heterostructures using angle-resolved photoemission spectroscopy. 1H-TaSe2 exhibits significant charge transfer and band hybridization at the interface, whereas 1 T-TaSe2 shows weak interactions with the substrate. The distinct interfacial interactions are attributed to the dual effects from the differences of the work functions as well as the relative interlayer distance between TaSe2 films and BLG substrate. The method demonstrated here provides a viable route towards interface engineering in a variety of transition-metal dichalcogenides that can be applied to future nano-devices with designed electronic properties.

Applying lattice strain to thin films, a critical factor to tailor their properties such as stabilizing a structural phase unstable at ambient pressure, generally necessitates heteroepitaxial growth to control the lattice mismatch with substrate. Therefore, while homoepitaxy, the growth of thin film on a substrate made of the same material, is a useful method to fabricate high‐quality thin films, its application to studying strain‐induced structural phases is limited. Contrary to this general belief, here the quasi‐homoepitaxial growth of Cs and Rb thin films is reported with substantial in‐plane compressive strain. This is achieved by utilizing the alkali‐metal layer existing in bulk crystal of kagome metals AV3Sb5 (A = Cs and Rb) as a structural template. The angle‐resolved photoemission spectroscopy measurements reveal the formation of metallic quantum well states and notable thickness‐dependent quasiparticle lifetime. Comparison with density functional theory calculations suggests that the obtained thin films crystalize in the face‐centered cubic structure, which is typically stable only under high pressure in bulk crystals. These findings provide a useful approach for synthesizing highly strained thin films by quasi‐homoepitaxy, and pave the way for investigating many‐body interactions in Fermi liquids with tunable dimensionality. [ABSTRACT FROM AUTHOR]

We investigate the electronic properties of a graphene and α-ruthenium trichloride (α-RuCl3) heterostructure using a combination of experimental techniques. α-RuCl3 is a Mott insulator and a Kitaev material. Its combination with graphene has gained increasing attention due to its potential applicability in novel optoelectronic devices. By using a combination of spatially resolved photoemission spectroscopy and low-energy electron microscopy, we are able to provide a direct visualization of the massive charge transfer from graphene to α-RuCl3, which can modify the electronic properties of both materials, leading to novel electronic phenomena at their interface. A measurement of the spatially resolved work function allows for a direct estimate of the interface dipole between graphene and α-RuCl3. Their strong coupling could lead to new ways of manipulating electronic properties of a two-dimensional heterojunction. Understanding the electronic properties of this structure is pivotal for designing next generation low-power optoelectronics devices.

Abstract Dimensional modifications play a crucial role in various applications, especially in the context of device miniaturization, giving rise to novel quantum phenomena. The many-body dynamics induced by dimensional modifications, including electron-electron, electron-phonon, electron-magnon and electron-plasmon coupling, are known to significantly affect the atomic and electronic properties of the materials. By reducing the dimensionality of orthorhombic CoSe2 and forming heterostructure with bilayer graphene using molecular beam epitaxy, we unveil the emergence of two types of phase transitions through angle-resolved photoemission spectroscopy and scanning tunneling microscopy measurements. We disclose that the 2 × 1 superstructure is associated with charge density wave induced by Fermi surface nesting, characterized by a transition temperature of 340 K. Additionally, another phase transition at temperature of 160 K based on temperature dependent gap evolution are observed with renormalized electronic structure induced by electron-boson coupling. These discoveries of the electronic and atomic modifications, influenced by electron-electron and electron-boson interactions, underscore that many-body physics play significant roles in understanding low-dimensional properties of non-van der Waals Co-chalcogenides and related heterostructures. Graphical Abstract

[Display omitted] α -Sn is an elemental topological material, whose topological phases can be tuned by strain and magnetic field. Such tunability offers a substantial potential for topological electronics. However, InSb substrates, commonly used to stabilize α -Sn allotrope, suffer from parallel conduction, restricting transport investigations and potential applications. Here, the successful MBE growth of high-quality α -Sn layers on insulating, hybrid (001) CdTe/GaAs substrates, with bulk electron mobility approaching 20000 cm2V−1s−1 is reported. The electronic properties of the samples are systematically investigated by independent complementary techniques, enabling thorough characterization of the 3D Dirac (DSM) and Weyl (WSM) semimetal phases induced by the strains and magnetic field, respectively. Magneto-optical experiments, corroborated with band structure modelling, provide an exhaustive description of the bulk states in the DSM phase. The modelled electronic structure is directly observed in angle-resolved photoemission spectroscopy, which reveals linearly dispersing bands near the Fermi level. The first detailed study of negative longitudinal magnetoresistance relates this effect to the chiral anomaly and, consequently, to the presence of WSM. Observation of the π Berry phase in Shubnikov-de Haas oscillations agrees with the topologically non-trivial nature of the investigated samples. Our findings establish α -Sn as an attractive topological material for exploring relativistic physics and future applications. [ABSTRACT FROM AUTHOR]

Dimensional modifications play a crucial role in various applications, especially in the context of device miniaturization, giving rise to novel quantum phenomena. The many-body dynamics induced by dimensional modifications, including electron-electron, electron-phonon, electron-magnon and electron-plasmon coupling, are known to significantly affect the atomic and electronic properties of the materials. By reducing the dimensionality of orthorhombic CoSe2 and forming heterostructure with bilayer graphene using molecular beam epitaxy, we unveil the emergence of two types of phase transitions through angle-resolved photoemission spectroscopy and scanning tunneling microscopy measurements. We disclose that the 2 × 1 superstructure is associated with charge density wave induced by Fermi surface nesting, characterized by a transition temperature of 340 K. Additionally, another phase transition at temperature of 160 K based on temperature dependent gap evolution are observed with renormalized electronic structure induced by electron-boson coupling. These discoveries of the electronic and atomic modifications, influenced by electron-electron and electron-boson interactions, underscore that many-body physics play significant roles in understanding low-dimensional properties of non-van der Waals Co-chalcogenides and related heterostructures. [ABSTRACT FROM AUTHOR]

Layered material TaS2 hosts multiple structural phases and exotic correlated quantum states, including charge density wave (CDW), superconductivity, quantum spin liquid, and Mott insulating state. Here, we synthesized TaS2 monolayers in H and T phases using the molecular beam epitaxial (MBE) method and studied their electronic structures via angle-resolved photo-emission spectroscopy (ARPES). We found that the H phase TaS2 (H-TaS2) monolayer is metallic, with an energy band crossing the Fermi level. In contrast, the T phase TaS2 (T-TaS2) monolayer shows an insulated energy gap at the Fermi level, while the normal calculated band structure implies it should be metallic without any band gap. However, by considering Hubbard interaction potential U, further density functional theory (DFT) calculation suggests that monolayer T-TaS2 could be a CDW Mott insulator, and the DFT+U calculation matches well with the ARPES result. More significantly, the temperature-dependent ARPES result indicates that the CDW Mott state in the T-TaS2 monolayer is more robust than its bulk counterpart and can persist at room temperature. Our results reveal that the dimensional effect can enhance the CDW Mott state and provide valuable insights for further exploring the exotic properties of monolayer TaS2. [ABSTRACT FROM AUTHOR]

Tunability of interfacial effects between two-dimensional (2D) crystals is crucial not only for understanding the intrinsic properties of each system, but also for designing electronic devices based on ultra-thin heterostructures. A prerequisite of such heterostructure engineering is the availability of 2D crystals with different degrees of interfacial interactions. In this work, we report a controlled epitaxial growth of monolayer TaSe2 with different structural phases, 1H and 1 T, on a bilayer graphene (BLG) substrate using molecular beam epitaxy, and its impact on the electronic properties of the heterostructures using angle-resolved photoemission spectroscopy. 1H-TaSe2 exhibits significant charge transfer and band hybridization at the interface, whereas 1 T-TaSe2 shows weak interactions with the substrate. The distinct interfacial interactions are attributed to the dual effects from the differences of the work functions as well as the relative interlayer distance between TaSe2 films and BLG substrate. The method demonstrated here provides a viable route towards interface engineering in a variety of transition-metal dichalcogenides that can be applied to future nano-devices with designed electronic properties. [ABSTRACT FROM AUTHOR]

Unconventional fermions in the immensely studied topological semimetals are the source for rich exotic topological properties. Here, using symmetry analysis and first-principles calculations, we propose the coexistence of multiple topological nodal structure in LaSb2, including topological nodal surfaces, nodal lines and in particular eightfold degenerate nodal points, which have been scarcely observed in a single material. Further, utilizing angle-resolved photoemission spectroscopy, we confirm the existence of nodal surfaces and eightfold degenerate nodal points in LaSb2. The intriguing multiple topological nodal structure might play a crucial role in giving rise to the large linear magnetoresistance. Our work renews the insights into the exotic topological phenomena in LaSb2. [ABSTRACT FROM AUTHOR]

The evolution of the physical properties of 2D material from monolayer limit to the bulk reveals unique consequences from dimension confinement and provides a distinct tuning knob for applications. Monolayer 1T'-phase transition metal dichalcogenides (1T'-TMDs) with ubiquitous quantum spin Hall (QSH) states are ideal 2D building blocks of various 3D topological phases. However, the stacking geometry has been previously limited to the bulk 1T'-WTe2 type. Here, the novel 2M-TMDs consisting of translationally stacked 1T'-monolayers are introduced as promising material platforms with tunable inverted bandgaps and interlayer coupling. By performing advanced polarization-dependent angle-resolved photoemission spectroscopy as well as first-principles calculations on the electronic structure of 2M-TMDs, a topology hierarchy is revealed: 2M-WSe2 , MoS2, and MoSe2 are weak topological insulators (WTIs), whereas 2M-WS2 is a strong topological insulator (STI). Further demonstration of topological phase transitions by tunning interlayer distance indicates that band inversion amplitude and interlayer coupling jointly determine different topological states in 2M-TMDs. It is proposed that 2M-TMDs are parent compounds of various exotic phases including topological superconductors and promise great application potentials in quantum electronics due to their flexibility in patterning with 2D materials.

Abstract Applying lattice strain to thin films, a critical factor to tailor their properties such as stabilizing a structural phase unstable at ambient pressure, generally necessitates heteroepitaxial growth to control the lattice mismatch with substrate. Therefore, while homoepitaxy, the growth of thin film on a substrate made of the same material, is a useful method to fabricate high‐quality thin films, its application to studying strain‐induced structural phases is limited. Contrary to this general belief, here the quasi‐homoepitaxial growth of Cs and Rb thin films is reported with substantial in‐plane compressive strain. This is achieved by utilizing the alkali‐metal layer existing in bulk crystal of kagome metals AV3Sb5 (A = Cs and Rb) as a structural template. The angle‐resolved photoemission spectroscopy measurements reveal the formation of metallic quantum well states and notable thickness‐dependent quasiparticle lifetime. Comparison with density functional theory calculations suggests that the obtained thin films crystalize in the face‐centered cubic structure, which is typically stable only under high pressure in bulk crystals. These findings provide a useful approach for synthesizing highly strained thin films by quasi‐homoepitaxy, and pave the way for investigating many‐body interactions in Fermi liquids with tunable dimensionality.

Ferromagnetic insulators (FMIs) are intriguing not only due to their rare nature, but also due to their potential applications in spintronics and various electronic devices. One of its key promising applications is based on an FMI-induced magnetic proximity effect, which can impose an effective time-reversal symmetry breaking on the target ultrathin layer to realize novel emergent phenomena. Here, we conduct systematic studies on thin film LaCoO3, an insulator known to be ferromagnet under tensile strain, with varying thicknesses, to establish it as an FMI platform to be integrated in heterostructures. The optimal thickness of the LaCoO3 layer, providing a smooth surface and robust ferromagnetism with large remanence, is determined. A heterostructure consisting of an ultrathin target layer (2 uc SrRuO3), the LaCoO3 FMI layer, and the La0.5Sr0.5CoO3 conducting layer has been fabricated and the angle-resolved photoemission spectroscopy measurement on the multi-layer system demonstrates a sharp Fermi edge and a well-defined Fermi surface without the charging effect. This demonstrates the feasibility of the proposed heterostructure using LaCoO3 thin film as the FMI layer, and further lays a groundwork to investigate the magnetic proximity induced phases in quantum materials. [ABSTRACT FROM AUTHOR]

In the past 5 years, there has been significant research interest in the intrinsic magnetic topological insulator family compounds MnBi2+2n Te4+3n (where n  = 0, 1, 2 ...). In particular, exfoliated thin films of MnBi2Te4 have led to numerous experimental breakthroughs, such as the quantum anomalous Hall effect, axion insulator phase and high-Chern number quantum Hall effect without Landau levels. However, despite extensive efforts, the energy gap of the topological surface states due to exchange magnetic coupling, which is a key feature of the characteristic band structure of the system, remains experimentally elusive. The electronic structure measured by using angle-resolved photoemission (ARPES) shows significant deviation from ab initio prediction and scanning tunneling spectroscopy measurements, making it challenging to understand the transport results based on the electronic structure. This paper reviews the measurements of the band structure of MnBi2+2n Te4+3n magnetic topological insulators using ARPES, focusing on the evolution of their electronic structures with temperature, surface and bulk doping and film thickness. The aim of the review is to construct a unified picture of the electronic structure of MnBi2+2n Te4+3n compounds and explore possible control of their topological properties. [ABSTRACT FROM AUTHOR]

A current key challenge in 2D materials is the realization of emergent quantum phenomena in hetero structures via controlling the moiré potential created by the periodicity mismatch between adjacent layers, as highlighted by the discovery of superconductivity in twisted bilayer graphene. Generally, the lattice structure of the original host material remains unchanged even after the moiré superlattice is formed. However, much less attention is paid for the possibility that the moiré potential can also modify the original crystal structure itself. Here, it is demonstrated that octahedral MoTe2 which is unstable in bulk is stabilized in a commensurate MoTe2/graphene hetero‐bilayer due to the moiré potential created between the two layers. It is found that the reconstruction of electronic states via the moiré potential is responsible for this stabilization, as evidenced by the energy‐gap opening at the Fermi level observed by angle‐resolved photoemission and scanning tunneling spectroscopies. The present results provide a fresh approach to realize novel 2D quantum phases by utilizing the moiré potential. [ABSTRACT FROM AUTHOR]

Quasi-one-dimensional materials offer an ideal playground to investigate weak topological insulators (WTIs) and higher-order topological insulators (HOTIs), since their characteristic boundary states emerge in the naturally cleaved surfaces. Utilizing laser-based angle-resolved photoemission spectroscopy (ARPES) and synchrotron-based nano-ARPES, we show evidence of a WTI phase in β-Bi4I4 and a HOTI phase in Bi4Br4. [ABSTRACT FROM AUTHOR]

Quantum well states (QWSs) can form at the surface or interfaces of materials with confinement potential. They have broad applications in electronic and optical devices such as high mobility electron transistor, photodetector, and quantum well laser. The properties of the QWSs are usually the key factors for the performance of the devices. However, direct visualization and manipulation of such states are, in general, challenging. In this work, by using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy/spectroscopy (STM/STS), we directly probe the QWSs generated on the vacuum interface of a narrow band gap semiconductor Nb2SiTe4. Interestingly, the position and splitting of QWSs could be easily manipulated via potassium (K) dosage onto the sample surface. Our results suggest Nb2SiTe4 to be an intriguing semiconductor system to study and engineer the QWSs, which has great potential in device applications.

The high-mobility conducting interface (CI) between LaAlO3 (LAO) and SrTiO3 (STO) has revealed many fascinating phenomena, including exotic magnetism and superconductivity. But, the formation mechanism of the CI has not been conclusively explained. Here, using in situ angle-resolved photoemission spectroscopy, we elucidated the mechanisms for the CI formation. In as-grown samples, we observed a built-in potential (Vbi) proportional to the polar LAO thickness starting from the first unit cell (UC) with CI formation appearing above 3 UCs. However, we found that the Vbi is removed by synchrotron ultraviolet (UV)-irradiation; The built-in potential is recovered by oxygen gas (O2(g))-exposure. Furthermore, after UV-irradiation, the CI appears even below 3UC of LAO. Our results demonstrate not only the Vbi-driven CI formation in as-grown LAO/STO, but also a new route to control of the interface state by UV lithographic patterning or other surface modification.

Vanadium disulfide (VS2) attracts elevated interests for its charge-density wave (CDW) phase transition, ferromagnetism, and catalytic reactivity, but the electronic structure of monolayer has not been well understood yet. Here we report synthesis of epitaxial 1T VS2 monolayer on bilayer graphene grown by molecular-beam epitaxy (MBE). Angle-resolved photoemission spectroscopy (ARPES) measurements reveal that Fermi surface with six elliptical pockets centered at the M points shows gap opening at low temperature. Temperature-dependence of the gap size suggests existence of CDW phase transition above room temperature. Our observations provide important evidence to understand the strongly correlated electron physics and the related surface catalytic properties in two-dimensional transition-metal dichalcogenides (TMDCs).

Intrinsic magnetic topological insulators offer low disorder and large magnetic band gaps for robust magnetic topological phases operating at higher temperatures. By controlling the layer thickness, emergent phenomena such as the quantum anomalous Hall (QAH) effect and axion insulator phases have been realized. These observations occur at temperatures significantly lower than the Néel temperature of bulk MnBi2Te4, and measurement of the magnetic energy gap at the Dirac point in ultrathin MnBi2Te4 has yet to be achieved. Critical to achieving the promise of this system is a direct measurement of the layer-dependent energy gap and verification of a temperature-dependent topological phase transition from a large band gap QAH insulator to a gapless TI paramagnetic phase. Here we utilize temperature-dependent angle-resolved photoemission spectroscopy to study epitaxial ultrathin MnBi2Te4. We directly observe a layer-dependent crossover from a 2D ferromagnetic insulator with a band gap greater than 780 meV in one septuple layer (1 SL) to a QAH insulator with a large energy gap (>70 meV) at 8 K in 3 and 5 SL MnBi2Te4. The QAH gap is confirmed to be magnetic in origin, as it becomes gapless with increasing temperature above 8 K.

Abstract A current key challenge in 2D materials is the realization of emergent quantum phenomena in hetero structures via controlling the moiré potential created by the periodicity mismatch between adjacent layers, as highlighted by the discovery of superconductivity in twisted bilayer graphene. Generally, the lattice structure of the original host material remains unchanged even after the moiré superlattice is formed. However, much less attention is paid for the possibility that the moiré potential can also modify the original crystal structure itself. Here, it is demonstrated that octahedral MoTe2 which is unstable in bulk is stabilized in a commensurate MoTe2/graphene hetero‐bilayer due to the moiré potential created between the two layers. It is found that the reconstruction of electronic states via the moiré potential is responsible for this stabilization, as evidenced by the energy‐gap opening at the Fermi level observed by angle‐resolved photoemission and scanning tunneling spectroscopies. The present results provide a fresh approach to realize novel 2D quantum phases by utilizing the moiré potential.

2D materials provide a rich platform to study novel physical phenomena arising from quantum confinement of charge carriers. Many of these phenomena are discovered by surface sensitive techniques, such as photoemission spectroscopy, that work in ultra‐high vacuum (UHV). Success in experimental studies of 2D materials, however, inherently relies on producing adsorbate‐free, large‐area, high‐quality samples. The method that yields 2D materials of highest quality is mechanical exfoliation from bulk‐grown samples. However, as this technique is traditionally performed in a dedicated environment, the transfer of samples into vacuum requires surface cleaning that might diminish the quality of the samples. In this article, a simple method for in situ exfoliation directly in UHV is reported, which yields large‐area, single‐layered films. Multiple metallic and semiconducting transition metal dichalcogenides are exfoliated in situ onto Au, Ag, and Ge. The exfoliated flakes are found to be of sub‐millimeter size with excellent crystallinity and purity, as supported by angle‐resolved photoemission spectroscopy, atomic force microscopy, and low‐energy electron diffraction. The approach is well‐suited for air‐sensitive 2D materials, enabling the study of a new suite of electronic properties. In addition, the exfoliation of surface alloys and the possibility of controlling the substrate‐2D material twist angle is demonstrated. [ABSTRACT FROM AUTHOR]

The helicity of three‐dimensional (3D) topological insulator surface states has drawn significant attention in spintronics owing to spin‐momentum locking where the carriers' spin is oriented perpendicular to their momentum. This property can provide an efficient method to convert charge currents into spin currents, and vice‐versa, through the Rashba–Edelstein effect. However, experimental signatures of these surface states to the spin‐charge conversion are extremely difficult to disentangle from bulk state contributions. Here, spin‐ and angle‐resolved photo‐emission spectroscopy, and time‐resolved THz emission spectroscopy are combined to categorically demonstrate that spin‐charge conversion arises mainly from the surface state in Bi1 − xSbx ultrathin films, down to few nanometers where confinement effects emerge. This large conversion efficiency is correlated, typically at the level of the bulk spin Hall effect from heavy metals, to the complex Fermi surface obtained from theoretical calculations of the inverse Rashba–Edelstein response. Both surface state robustness and sizeable conversion efficiency in epitaxial Bi1 − xSbx thin films bring new perspectives for ultra‐low power magnetic random‐access memories and broadband THz generation. [ABSTRACT FROM AUTHOR]

The newly discovered ternary chalcogenide superconductor Bi2Rh3Se2 has attracted growing attention, which provides an opportunity to explore the interplay between charge density wave (CDW) order and superconductivity. However, whether the phase transition around 240 K can be attributed to the formation of CDW remains controversial. To help resolve the debate, we study the electronic structure of Bi2Rh3Se2 by angle-resolved photoemission spectroscopy, focusing on the nature of its high-temperature phase transition around 240 K. Our measurements demonstrate that the phase transition at 240 K is a second-order CDW phase transition. Our results reveal (i) a 2 × 2 CDW order in Bi2Rh3Se2, accompanied by the reconstruction of electronic structure, such as band folding, band splitting, and opening of CDW gaps at and away from the Fermi level; (ii) the existence of electron-boson coupling, which is manifested as an apparent kink and peak-dip-hump structure in dispersion. Our observations thus enable us to shed light on the nature of CDW order and superconductivity in Bi2Rh3Se2. [ABSTRACT FROM AUTHOR]

Abstract 2D materials provide a rich platform to study novel physical phenomena arising from quantum confinement of charge carriers. Many of these phenomena are discovered by surface sensitive techniques, such as photoemission spectroscopy, that work in ultra‐high vacuum (UHV). Success in experimental studies of 2D materials, however, inherently relies on producing adsorbate‐free, large‐area, high‐quality samples. The method that yields 2D materials of highest quality is mechanical exfoliation from bulk‐grown samples. However, as this technique is traditionally performed in a dedicated environment, the transfer of samples into vacuum requires surface cleaning that might diminish the quality of the samples. In this article, a simple method for in situ exfoliation directly in UHV is reported, which yields large‐area, single‐layered films. Multiple metallic and semiconducting transition metal dichalcogenides are exfoliated in situ onto Au, Ag, and Ge. The exfoliated flakes are found to be of sub‐millimeter size with excellent crystallinity and purity, as supported by angle‐resolved photoemission spectroscopy, atomic force microscopy, and low‐energy electron diffraction. The approach is well‐suited for air‐sensitive 2D materials, enabling the study of a new suite of electronic properties. In addition, the exfoliation of surface alloys and the possibility of controlling the substrate‐2D material twist angle is demonstrated.

Abstract The helicity of three‐dimensional (3D) topological insulator surface states has drawn significant attention in spintronics owing to spin‐momentum locking where the carriers' spin is oriented perpendicular to their momentum. This property can provide an efficient method to convert charge currents into spin currents, and vice‐versa, through the Rashba–Edelstein effect. However, experimental signatures of these surface states to the spin‐charge conversion are extremely difficult to disentangle from bulk state contributions. Here, spin‐ and angle‐resolved photo‐emission spectroscopy, and time‐resolved THz emission spectroscopy are combined to categorically demonstrate that spin‐charge conversion arises mainly from the surface state in Bi1 − xSbx ultrathin films, down to few nanometers where confinement effects emerge. This large conversion efficiency is correlated, typically at the level of the bulk spin Hall effect from heavy metals, to the complex Fermi surface obtained from theoretical calculations of the inverse Rashba–Edelstein response. Both surface state robustness and sizeable conversion efficiency in epitaxial Bi1 − xSbx thin films bring new perspectives for ultra‐low power magnetic random‐access memories and broadband THz generation.

Plumbene, with a structure similar to graphene, is expected to possess a strong spin–orbit coupling and thus enhances its superconducting critical temperature (Tc). In this work, a buckled plumbene‐Au Kagome superstructure grown by depositing Au on Pb(111) is investigated. The superconducting gap monitored by temperature‐dependent scanning tunneling microscopy/spectroscopy shows that the buckled plumbene‐Au Kagome superstructure not only has an enhanced Tc with respect to that of a monolayer Pb but also possesses a higher value than what owned by a bulk Pb substrate. By combining angle‐resolved photoemission spectroscopy with density functional theory, the monolayer Au‐intercalated low‐buckled plumbene sandwiched between the top Au Kagome layer and the bottom Pb(111) substrate is confirmed and the electron–phonon coupling‐enhanced superconductivity is revealed. This work demonstrates that a buckled plumbene‐Au Kagome superstructure can enhance superconducting Tc and Rashba effect, effectively triggering the novel properties of a plumbene. [ABSTRACT FROM AUTHOR]

First-principles calculations for underdoped La2−xSrxCuO4 (LSCO) have revealed a Fermi surface consisting of spin-triplet (KS) particles at the antinodal Fermi-pockets and spin-singlet (SS) particles at the nodal Fermi-arcs in the presence of AF local order. By performing a unique method of calculating the electronic-spin state of overdoped LSCO and by measurement of the spin-correlation length by neutron inelastic scattering, the origin of the phase-diagram, including the pseudogap phase in the high temperature superconductor, Sr-doped copper-oxide LSCO, has been elucidated. We have theoretically solved the long-term problem as to why the angle-resolved photoemission spectroscopy (ARPES) has not been able to observe Fermi pockets in the Fermi surface of LSCO. As a result, we show that the pseudogap region is bounded below the characteristic temperature T*(x) and above the superconducting transition temperature Tc(x) in the T vs. x phase diagram, where both the AF order and the KS particles in the Fermi pockets vanish at T*(x), whilst KS particles contribute to d-wave superconductivity below Tc. We also show that the relationship T*(xc) = Tc(xc) holds at xc = 0.30, which is consistent with ARPES experiments. At T*(x), a phase transition occurs from the pseudogap phase to an unusual metallic phase in which only the SS particles exist. [ABSTRACT FROM AUTHOR]

[Display omitted] The itinerant ferromagnetism can be induced by a van Hove singularity (VHS) with a divergent density of states at Fermi level. Utilizing the giant magnified dielectric constant ε r of SrTiO 3 (111) substrate with cooling, here we successfully manipulated the VHS in the epitaxial monolayer (ML) 1T-VSe 2 film approaching to Fermi level via the large interfacial charge transfer, and thus induced a two-dimensional (2D) itinerant ferromagnetic state below 3.3 K. Combining the direct characterization of the VHS structure via angle-resolved photoemission spectroscopy (ARPES), together with the theoretical analysis, we ascribe the manipulation of VHS to the physical origin of the itinerant ferromagnetic state in ML 1T-VSe 2. Therefore, we further demonstrated that the ferromagnetic state in the 2D system can be controlled through manipulating the VHS by engineering the film thickness or replacing the substrate. Our findings clearly evidence that the VHS can serve as an effective manipulating degree of freedom for the itinerant ferromagnetic state, expanding the application potentials of 2D magnets for the next-generation information technology. [ABSTRACT FROM AUTHOR]

Developing reliable methods for modulating the electronic structure of the 2D electron gas (2DEG) in SrTiO3 is crucial for utilizing its full potential and inducing novel properties. Herein, it is shown that relatively simple surface preparation reconstructs the 2DEG at the SrTiO3 (STO) surface, leading to a Lifshitz‐like transition. Combining experimental methods, such as angle‐resolved photoemission spectroscopy (ARPES) and X‐ray photoemission spectroscopy with ab initio calculations, that the modulation of the surface band structures can be effectively achieved via transforming the chemical composition at the atomic scale is found. In addition, ARPES experiments demonstrate that vacuum ultraviolet light can be efficiently employed to alter the band renormalization of the 2DEG system and control the electron‐phonon interaction. This study provides a robust and straightforward route to stabilize and tune the low‐dimensional electronic structure via the chemical degeneracy of the STO surface. [ABSTRACT FROM AUTHOR]

Ferroelectric materials have received great attention in the field of data storage, benefiting from their exotic transport properties. Among these materials, the two-dimensional (2D) In2Se3 has been of particular interest because of its ability to exhibit both in-plane and out-of-plane ferroelectricity. In this article, we realized the molecular beam epitaxial (MBE) growth of β–In2Se3 films on bilayer graphene (BLG) substrates with precisely controlled thickness. Combining in situ scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES) measurements, we found that the four-monolayer β–In2Se3 is a semiconductor with a (9 × 1) reconstructed superlattice. In contrast, the monolayer β–In2Se3/BLG heterostructure does not show any surface reconstruction due to the interfacial interaction and moiré superlattice, which instead results in a folding Dirac cone at the center of the Brillouin zone. In addition, we found that the band gap of In2Se3 film decreases after potassium doping on its surface, and the valence band maximum also shifts in momentum after surface potassium doping. The successful growth of high-quality β–In2Se3 thin films would be a new platform for studying the 2D ferroelectric heterostructures and devices. The experimental results on the surface reconstruction and band structures also provide important information on the quantum confinement and interfacial effects in the epitaxial β–In2Se3 films. [ABSTRACT FROM AUTHOR]

Angle‐resolved photoemission spectroscopy (ARPES) is performed on single‐crystalline tin(II) sulfide (SnS) over a wide energy range (from Fermi level to −10 eV) using four measurement geometries with different excitation light polarizations and sample rotation angles. Based on the different symmetries of the atomic orbitals with respect to the mirror plane, the contribution of each atomic orbital of the constituent elements to the SnS valence band is determined. The results obtained agree with those of first‐principles calculations. Experimental results indicate that at the top of the valence band, the S 3py and 3pz contributions are strong near the Z and Γ points, respectively. Meanwhile, in the same region, the S 3px contribution is minimal and is concentrated at −2 eV lower than that of the valence band maximum. Although ARPES measurements are performed at different geometries, direct comparisons of the obtained measurements with calculation results are rarely conducted over such a wide energy range. This study is an effective example of experimental identification of the electronic band structures. [ABSTRACT FROM AUTHOR]

The resistance of a conventional insulator diverges as temperature approaches zero. The peculiar low-temperature resistivity saturation in the 4f Kondo insulator (KI) SmB6 has spurred proposals of a correlation-driven topological Kondo insulator (TKI) with exotic ground states. However, the scarcity of model TKI material families leaves difficulties in disentangling key ingredients from irrelevant details. Here we use angle-resolved photoemission spectroscopy (ARPES) to study FeSb2, a correlated d-electron KI candidate that also exhibits a low-temperature resistivity saturation. On the (010) surface, we find a rich assemblage of metallic states with two-dimensional dispersion. Measurements of the bulk band structure reveal band renormalization, a large temperature-dependent band shift, and flat spectral features along certain high-symmetry directions, providing spectroscopic evidence for strong correlations. Our observations suggest that exotic insulating states resembling those in SmB6 and YbB12 may also exist in systems with d instead of f electrons.

Abstract Plumbene, with a structure similar to graphene, is expected to possess a strong spin–orbit coupling and thus enhances its superconducting critical temperature (Tc). In this work, a buckled plumbene‐Au Kagome superstructure grown by depositing Au on Pb(111) is investigated. The superconducting gap monitored by temperature‐dependent scanning tunneling microscopy/spectroscopy shows that the buckled plumbene‐Au Kagome superstructure not only has an enhanced Tc with respect to that of a monolayer Pb but also possesses a higher value than what owned by a bulk Pb substrate. By combining angle‐resolved photoemission spectroscopy with density functional theory, the monolayer Au‐intercalated low‐buckled plumbene sandwiched between the top Au Kagome layer and the bottom Pb(111) substrate is confirmed and the electron–phonon coupling‐enhanced superconductivity is revealed. This work demonstrates that a buckled plumbene‐Au Kagome superstructure can enhance superconducting Tc and Rashba effect, effectively triggering the novel properties of a plumbene.

Nodal-line semimetals (NLSs) represent a new type of topological semimetallic phase beyond Weyl and Dirac semimetals in the sense that they host closed loops or open curves of band degeneracies in the Brillouin zone. Parallel to the classification of type-I and type-II Weyl semimetals, there are two types of NLSs. The type-I NLS phase has been proposed and realized in many compounds, whereas the exotic type-II NLS phase that strongly violates Lorentz symmetry has remained elusive. First-principles calculations show that Mg3Bi2 is a material candidate for the type-II NLS. The band crossing is close to the Fermi level and exhibits the type-II nature of the nodal line in this material. Spin-orbit coupling generates only a small energy gap (≈35 meV) at the nodal points and does not negate the band dispersion of Mg3Bi2 that yields the type-II nodal line. Based on this prediction, Mg3Bi2 single crystals are synthesized and the presence of the type-II nodal lines in the material is confirmed. The angle-resolved photoemission spectroscopy measurements agree well with the first-principles results below the Fermi level and thus strongly suggest Mg3Bi2 as an ideal material platform for studying the as-yet unstudied properties of type-II nodal-line semimetals.

We report on in situ investigation of Au intercalation of different zero-layer graphene surface reconstructions of 6 H -SiC(0001): (3 × 3) R 3 0 ∘ + (6 3 × 6 3) R 3 0 ∘ , (6 3 × 6 3) R 3 0 ∘ + (5 × 5) R 0 ∘ , (6 3 × 6 3) R 3 0 ∘ + (5 × 5) R 0 ∘ +Gr. We show that the most appropriate reconstruction for graphene formation via Au intercalation is a one with some fraction of initial graphene monolayer. A well-ordered epitaxial Au(111) islands on the zero-layer graphene were revealed with the same crystallographic orientation as the SiC surface. Ab initio calculations approve that the value of Rashba splitting in graphene increases with the density of Au atoms per unit cell and with the reduction of average distance between Au and graphene. [Display omitted] • ZLG with some graphene fraction is the most efficient for Au atoms intercalation. • Well-ordered epitaxial Au(111) islands form on the ZLG surface. • Rashba splitting depends on the density of Au atoms and their distance from graphene. [ABSTRACT FROM AUTHOR]

Using high resolution angle-resolved photoemission spectroscopy, we systematically investigate the electronic structure of Td-WTe2, which has attracted substantial research attention due to its diverse and fascinating properties, especially the predicted type-II topological Weyl semimetal (TWS) phase. The observed significant lattice contraction and the fact that our ARPES measurements are well reproduced by our ab initio calculations under reduced lattice constants support the theoretical prediction of a type-II TWS phase in Td-WTe2 at temperatures below 10 K. We also investigate the evolution of the electronic structure of Td-WTe2 and realize two-stage Lifshitz transitions induced by temperature regulation and surface modification, respectively. Our results not only shed light on the understanding of the electronic structure of Td-WTe2, but also provide a promising method to manipulate the electronic structures and physical properties of the type-II TWS Td-XTe2.

Using high resolution angle-resolved photoemission spectroscopy, we systematically investigate the electronic structure of Td-WTe2, which has attracted substantial research attention due to its diverse and fascinating properties, especially the predicted type-II topological Weyl semimetal (TWS) phase. The observed significant lattice contraction and the fact that our ARPES measurements are well reproduced by our ab initio calculations under reduced lattice constants support the theoretical prediction of a type-II TWS phase in Td-WTe2 at temperatures below 10 K. We also investigate the evolution of the electronic structure of Td-WTe2 and realize two-stage Lifshitz transitions induced by temperature regulation and surface modification, respectively. Our results not only shed light on the understanding of the electronic structure of Td-WTe2, but also provide a promising method to manipulate the electronic structures and physical properties of the type-II TWS Td-XTe2.

2D layered germanium selenide (GeSe) material possesses in‐plane anisotropy because of low‐symmetry crystal structure with a new degree of freedom for enhanced optical and electronic properties. However, their systematic vibrational and electronics properties are still under the scope to study. Herein, the vibrational properties of GeSe sheets are studied by Raman spectroscopy. Whereas, the temperature‐dependent electronic band structure is studied using angle‐resolved photoemission spectroscopy (ARPES) combined with density functional theory calculations. Moreover, the field‐effect transistor (FET) is fabricated on a few‐layer GeSe with high performance. The vibrational modes B3g1 and Ag1 demonstrates linear softening as the temperature increases, with temperature coefficient value associated by anharmonic phonon–phonon/electron coupling. Besides, the enhanced dielectric screening effect of long‐range Coulomb and interlayer interaction is observed from bulk to monolayer. Similarly, ARPES results further show Fermi level movement toward the valance band as increased temperature represents hole doping to pining the Fermi level, which indicates superior carrier concentration for electronic properties. The fabricated FET device on six layers GeSe exhibits high carrier mobility of 52.89 cm2 V−1 s−1 with an on/off ratio above 4 × 105 at room temperature, while it decreased below the room temperature. Our results provide the important figure of merit for GeSe‐based novel nanoelectronic and thermoelectric devices. [ABSTRACT FROM AUTHOR]

Recently, unconventional antiferromagnets that enable the spin splitting (SS) of electronic states have been theoretically proposed and experimentally realized, where the magnetic sublattices containing moments pointing at different directions are connected by a novel set of symmetries. Such SS is substantial, k-dependent, and independent of the spin-orbit coupling (SOC) strength, making these magnets promising materials for antiferromagnetic spintronics. Here, combined with angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, a systematic study on CrSb, a metallic spin-split antiferromagnet candidate with Néel temperature T N = 703 K, is conducted. The data reveal the electronic structure of CrSb along both out-of-plane and in-plane momentum directions, rendering an anisotropic k-dependent SS that agrees well with the calculational results. The magnitude of such SS reaches up to at least 0.8 eV at non-high-symmetry momentum points, which is significantly higher than the largest known SOC-induced SS. This compound expands the choice of materials in the field of antiferromagnetic spintronics and is likely to stimulate subsequent investigations of high-efficiency spintronic devices that are functional at room temperature., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

In most charge density wave (CDW) systems of different material classes, ranging from traditional correlated systems in low-dimension to recent topological systems with Kagome lattice, superconductivity emerges when the system is driven toward the quantum critical point (QCP) of CDW via external parameters of doping and pressure. Despite this rather universal trend, the essential hinge between CDW and superconductivity has not been established yet. Here, the evidence of coupling between electron and CDW fluctuation is reported, based on a temperature- and intercalation-dependent kink in the angle-resolved photoemission spectra of 2H-Pd x TaSe 2 . Kinks are observed only when the system is in the CDW phase, regardless of whether a long- or short-range order is established. Notably, the coupling strength is enhanced upon long-range CDW suppression, albeit the coupling energy scale is reduced. Interestingly, the estimation of the superconducting critical temperature by incorporating the observed coupling characteristics into McMillan's equation yields results closely resembling the known values of the superconducting dome. The results thus highlight a compelling possibility that this new coupling mediates Cooper pairs, which provides new insights into the competing relationship not only for CDW but also for other competing orders., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Structural topology and symmetry of a two-dimensional (2D) network play pivotal roles in defining its electrical properties and functionalities. Here, a binary buckled honeycomb lattice with C 3v symmetry, which naturally hosts topological Dirac fermions and out-of-plane polarity, is proposed. It is successfully achieved in a group IV-V compound, namely monolayer SiP epitaxially grown on Ag(111) surface. Combining first-principles calculations with angle-resolved photoemission spectroscopy, the degeneration of the Dirac nodal lines to points due to the broken horizonal mirror symmetry is elucidated. More interesting, the SiP monolayer manifests metallic nature, which is mutually exclusive with polarity in conventional materials. It is further found that the out-of-plane polarity is strongly suppressed by the metallic substrate. This study not only represents a breakthrough of realizing intrinsic polarity in 2D metallic material via ingenious design but also provides a comprehensive understanding of the intricate interplay of many exotic low-dimensional quantum phenomena., (© 2024 Wiley‐VCH GmbH.)