Angle-resolved Photoemission Spectroscopy Measurements Research Articles

Hole-Carrier-Dominant Transport in 2D Single-Crystal Copper.

In 2D noble metals like copper, the carrier scattering at grain boundaries has obscured the intrinsic nature of electronic transport. However, it is demonstrated that the intrinsic nature of transport by hole carriers in 2D copper can be revealed by growing thin films without grain boundaries. As even a slight deviation from the twin boundary is perceived as grain boundaries by electrons, it is only through the thorough elimination of grain boundaries that the hidden hole-like attribute of 2D single-crystal copper can be unmasked. Two types of Fermi surfaces, a large hexagonal Fermi surface centered at the zone center and the triangular Fermi surface around the zone corner, tightly matching to the calculated Fermi surface topology, confirmed by angle-resolved photoemission spectroscopy (ARPES) measurements and vivid nonlinear Hall effects of the 2D single-crystal copper account for the presence of hole carriers experimentally. This breakthrough suggests the potential to manipulate the majority carrier polarity in metals by means of grain boundary engineering in a 2D geometry.

Robustness of linear bands in epitaxial planar silicene heterostructure against surface doping

In this study, we investigate the electronic structure of epitaxial planar silicene heterostructure grown on ultrathin gold films on the Si(111) substrates, covered by 0.1 monolayer of silver, antimony and lead. Angle-Resolved Photoemission Spectroscopy measurements reveal that the electronic structure of planar silicene, that shows bands with linear dispersion, remains largely unaffected by the presence of these dopants, with only a slight energy shift observed in the case of antimony. Density functional theory calculations corroborate these experimental observations, confirming the robustness of the epitaxial planar silicene heterostructure against surface doping. The results suggest that the intrinsic electronic properties of planar silicene are well-protected against surface contamination.

Quasi-Homoepitaxial Growth of Highly Strained Alkali-Metal Ultrathin Films on Kagome Superconductors.

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.

Emergence of two distinct phase transitions in monolayer CoSe2 on graphene

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 Two different pseudo-gaps and corresponding phase transitions are observed in monolayer orthorhombic CoSe2 grown on graphene substrates.

Unraveling electronic origins for boosting thermoelectric performance of p-type (Bi,Sb)2Te3.

P-type Bi2-xSbxTe3 compounds are crucial for thermoelectric applications at room temperature, with Bi0.5Sb1.5Te3 demonstrating superior performance, attributed to its maximum density-of-states effective mass (m*). However, the underlying electronic origin remains obscure, impeding further performance optimization. Herein, we synthesized high-quality Bi2-xSbxTe3 (00 l) films and performed comprehensive angle-resolved photoemission spectroscopy (ARPES) measurements and band structure calculations to shed light on the electronic structures. ARPES results directly evidenced that the band convergence along the [Formula: see text]-[Formula: see text] direction contributes to the maximum m* of Bi0.5Sb1.5Te3. Moreover, strategic manipulation of intrinsic defects optimized the hole density of Bi0.5Sb1.5Te3, allowing the extra valence band along [Formula: see text]-[Formula: see text] to contribute to the electrical transport. The synergy of the above two aspects documented the electronic origins of the Bi0.5Sb1.5Te3's superior performance that resulted in an extraordinary power factor of ~5.5 milliwatts per meter per square kelvin. The study offers valuable guidance for further performance optimization of p-type Bi2-xSbxTe3.

Spin-orbit-splitting-driven nonlinear Hall effect in NbIrTe4

The Berry curvature dipole (BCD) serves as a one of the fundamental contributors to emergence of the nonlinear Hall effect (NLHE). Despite intense interest due to its potential for new technologies reaching beyond the quantum efficiency limit, the interplay between BCD and NLHE has been barely understood yet in the absence of a systematic study on the electronic band structure. Here, we report NLHE realized in NbIrTe4 that persists above room temperature coupled with a sign change in the Hall conductivity at 150 K. First-principles calculations combined with angle-resolved photoemission spectroscopy (ARPES) measurements show that BCD tuned by the partial occupancy of spin-orbit split bands via temperature is responsible for the temperature-dependent NLHE. Our findings highlight the correlation between BCD and the electronic band structure, providing a viable route to create and engineer the non-trivial Hall effect by tuning the geometric properties of quasiparticles in transition-metal chalcogen compounds.

Hidden non-collinear spin-order induced topological surface states

Rare-earth monopnictides are a family of materials simultaneously displaying complex magnetism, strong electronic correlation, and topological band structure. The recently discovered emergent arc-like surface states in these materials have been attributed to the multi-wave-vector antiferromagnetic order, yet the direct experimental evidence has been elusive. Here we report observation of non-collinear antiferromagnetic order with multiple modulations using spin-polarized scanning tunneling microscopy. Moreover, we discover a hidden spin-rotation transition of single-to-multiple modulations 2 K below the Néel temperature. The hidden transition coincides with the onset of the surface states splitting observed by our angle-resolved photoemission spectroscopy measurements. Single modulation gives rise to a band inversion with induced topological surface states in a local momentum region while the full Brillouin zone carries trivial topological indices, and multiple modulation further splits the surface bands via non-collinear spin tilting, as revealed by our calculations. The direct evidence of the non-collinear spin order in NdSb not only clarifies the mechanism of the emergent topological surface states, but also opens up a new paradigm of control and manipulation of band topology with magnetism.

Emergence of quantum confinement in topological kagome superconductor CsV3Sb5

Quantum confinement is a restriction on the motion of electrons in a material to specific region, resulting in discrete energy levels rather than continuous energy bands. In certain materials, quantum confinement could dramatically reshape the electronic structure and properties of the surface with respect to the bulk. Here, in the recently discovered kagome superconductors CsV3Sb5, we unveil the dominant role of quantum confinement in determining their surface electronic structure. Combining angle-resolved photoemission spectroscopy (ARPES) measurement and density-functional theory simulation, we report the observations of two-dimensional quantum well states due to the confinement of bulk electron pocket and Dirac cone to the nearly isolated surface layer. The theoretical calculations on the slab model also suggest that the ARPES observed spectra are almost entirely contributed by the top two layers. Our results not only explain the disagreement of band structures between the recent experiments and calculations, but also suggest an equally important role played by quantum confinement, together with strong correlation and band topology, in shaping the electronic properties of this material.

Revealing the temperature-driven Lifshitz transition in p-type Mg3Sb2-based thermoelectric materials

The manipulation of native atomic defects and their thermal excitations plays vital roles in the thermoelectric performance of Mg3Sb2-based materials. While native defects manipulation has been intensively studied in p-type Mg3Sb2, there exists interesting unsolved issue regarding the abnormal semiconducting electrical behavior in most of samples. In this work, high quality Mg3Sb2 and Mg3Bi2 (00l) films are fabricated by molecular beam epitaxy technique, while variable temperature angle-resolved photoemission spectroscopy and scanning tunneling spectroscopy measurements are utilized for resolving the aforementioned issue. The thermal excitation of Mg interstitials (the electron donor) results in an obvious downshift of valence bands with rising temperature in both the p-type Mg3Sb2 and Mg3Bi2. Meanwhile, the interesting temperature-driven Lifshitz transition is discovered in the p-type Mg3Sb2, as indicated by the change of Fermi surface topology. Above the Lifshitz transition temperature, the Fermi level of p-type Mg3Sb2 will enter the bandgap, which leads to the abnormal semiconducting electrical behavior. This work discloses the excitation of native defects and temperature-driven Lifshitz transition, which are the main causes for the anomalies in electrical transport of p-type Mg3Sb2-based materials, and also provides valuable insights for further improving their thermoelectric performance.

Tunable positions of Weyl nodes via magnetism and pressure in the ferromagnetic Weyl semimetal CeAlSi

The noncentrosymmetric ferromagnetic Weyl semimetal CeAlSi with simultaneous space-inversion and time-reversal symmetry breaking provides a unique platform for exploring novel topological states. Here, by employing multiple experimental techniques, we demonstrate that ferromagnetism and pressure can serve as efficient parameters to tune the positions of Weyl nodes in CeAlSi. At ambient pressure, a magnetism-facilitated anomalous Hall/Nernst effect (AHE/ANE) is uncovered. Angle-resolved photoemission spectroscopy (ARPES) measurements demonstrated that the Weyl nodes with opposite chirality are moving away from each other upon entering the ferromagnetic phase. Under pressure, by tracing the pressure evolution of AHE and band structure, we demonstrate that pressure could also serve as a pivotal knob to tune the positions of Weyl nodes. Moreover, multiple pressure-induced phase transitions are also revealed. These findings indicate that CeAlSi provides a unique and tunable platform for exploring exotic topological physics and electron correlations, as well as catering to potential applications, such as spintronics.

Efficient Hydrogen Evolution Reaction in 2H-MoS2 Basal Planes Enhanced by Surface Electron Accumulation

An innovative strategy has been developed to activate the basal planes in molybdenum disulfide (MoS2) to improve their electrocatalytic activity by controlling surface electron accumulation (SEA) through aging, annealing, and nitrogen-plasma treatments. The optimal hydrogen evolution reaction (HER) performance was obtained on the surface treated with nitrogen-plasma for 120 s. An overpotential of 0.20 V and a Tafel slope of 120 mV dec−1 were achieved for the optimized condition. The angle-resolved photoemission spectroscopy measurement confirmed the HER efficiency enhanced by the SEA conjugated with the sulfur vacancy active sites in the MoS2 basal planes. This study provides new insight into optimizing MoS2 catalysts for energy applications.

Emergent Dirac Fermions in Epitaxial Planar Silicene Heterostructure.

Silicene, a single layer of Si atoms, shares many remarkable electronic properties with graphene. So far, silicene has been synthesized in its epitaxial form on a few surfaces of solids. Thus, the problem of silicene-substrate interaction appears, which usually depresses the original electronic behavior but may trigger properties superior to those of bare components. We report the direct observation of robust Dirac-dispersed bands in epitaxial silicene grown on Au(111) films deposited on Si(111). By performing in-depth angle-resolved photoemission spectroscopy measurements, we reveal three pairs of one-dimensional bands with linear dispersion running in three different directions of an otherwise two-dimensional system. By combining these results with first-principles calculations, we explore the nature of these bands and point to strong interaction between subsystems forming a complex Si-Au heterostructure. These findings emphasize the essential role of interfacial coupling and open a unique materials platform for exploring exotic quantum phenomena and applications in future-generation nanoelectronics.

Ferromagnetic insulating substrate for magnetic proximity studies: LaCoO3thin film.

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 LaCoO3layer, providing a smooth surface and robust ferromagnetism with large remanence, is determined. A heterostructure consisting of an ultrathin target layer (2 uc SrRuO3), the LaCoO3FMI layer, and the La0.5Sr0.5CoO3conducting 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 LaCoO3thin film as the FMI layer, and further lays a groundwork to investigate the magnetic proximity induced phases in quantum materials.

Topological electronic structure and spin texture of quasi-one-dimensional higher-order topological insulator Bi4Br4

The notion of topological insulators (TIs), characterized by an insulating bulk and conducting topological surface states, can be extended to higher-order topological insulators (HOTIs) hosting gapless modes localized at the boundaries of two or more dimensions lower than the insulating bulk. In this work, by performing high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements with submicron spatial and spin resolution, we systematically investigate the electronic structure and spin texture of quasi-one-dimensional (1D) HOTI candidate Bi4Br4. In contrast to the bulk-state-dominant spectra on the (001) surface, we observe gapped surface states on the (100) surface, whose dispersion and spin-polarization agree well with our ab-initio calculations. Moreover, we reveal in-gap states connecting the surface valence and conduction bands, which is a signature of the hinge states inside the (100) surface gap. Our findings provide compelling evidence for the HOTI phase of Bi4Br4. The identification of the higher-order topological phase promises applications based on 1D spin-momentum locked current in electronic and spintronic devices.

Identification of electronic dimensionality reduction in semiconductor quantum well structures

Two-dimensional (2D) systems, such as high-temperature superconductors, surface states of topological insulators, and layered materials, have been intensively studied using vacuum-ultraviolet (VUV) angle-resolved photoemission spectroscopy (ARPES). In semiconductor films (heterostructures), quantum well (QW) states arise due to electron/hole accumulations at the surface (interface). The quantized states due to quantum confinement can be observed by VUV-ARPES, while the periodic intensity modulations along the surface normal (kz) direction of these quantized states are also observable by varying incident photon energy, resembling three-dimensional (3D) band dispersion. We have conducted soft X-ray (SX) ARPES measurements on thick and ultrathin III-V semiconductor InSb(001) films to investigate the electronic dimensionality reduction in semiconductor QWs. In addition to the dissipation of the kz dispersion, the SX-ARPES observations demonstrate the changes of the symmetry and periodicity of the Brillouin zone in the ultrathin film as 2D QW compared with these of the 3D bulk one, indicating the electronic dimensionality reduction of the 3D bulk band dispersion caused by the quantum confinement. The results provide a critical diagnosis using SX-ARPES for the dimensionality reduction in semiconductor QW structures.

Intrinsically large effective mass and multi-valley band characteristics of n-type Bi2[sbnd]Bi2Te3 superlattice-like films

Thermoelectric superlattices are expected to decouple the strong correlation between various thermoelectric parameters, and are an important strategy for excellent thermoelectric performances. The superlattices of (Bi2)m(Bi2Te3)n homologous series are well-known for low lattice thermal conductivity and intriguing topological surface states. However, the impacts of electronic structure on the thermoelectric performance were still not well-understood in (Bi2)m(Bi2Te3)n. To cope with this issue, Bi2Bi2Te3 superlattice-like films with adjustable Bi2/(Bi2+Bi2Te3) molar ratio (R) were successfully fabricated by the molecular beam epitaxy technique. Angle-resolved photoemission spectroscopy measurements combined with theoretical calculations revealed the conduction band evolution from single-valley to multi-valley as R ≥ 0.30, leading to intrinsically high carrier effective mass and improved thermoelectric power factor. Also, the superlattice film (R = 0.46) with the structure close to Bi4Te3 possesses the topological surface state feature around the high symmetry point. As a result of the high effective mass of 3.9 m0 and very high electron density of 2.31 × 1021 cm−3, the film with R = 0.46 acquired the highest power factor of 1.49 mW·m−1·K−2 at 420 K, outperforming that of other (Bi2)m(Bi2Te3)n superlattices. This work lays an essential foundation on understanding the electronic structure and further improving thermoelectric performances of (Bi2)m(Bi2Te3)n homologous series.

Selective Control of Phases and Electronic Structures of Monolayer TaTe2.

Transition metal dichalcogenide (TMDC) films exhibit rich phases and superstructures, which can be controlled by the growth conditions as well as post-growth annealing treatment. Here, the selective growth of monolayer TaTe2 films with different phases as well as superstructures using molecular beam epitaxy (MBE) is reported. Monolayer 1H-TaTe2 and 1T-TaTe2 films can be selectively controlled by varying the growth temperature, and their different electronic structures are revealed through the combination of angle-resolved photoemission spectroscopy measurements (ARPES) and first-principles calculations. Moreover, post-growth annealing of the 1H-TaTe2 film further leads to a transition from a superstructure to a new 2 × 2 superstructure, where two gaps are observed in the electronic structure and persist up to room temperature. First-principles calculations reveal the role of the phonon instability in the formation of superstructures and the effect of local atomic distortions on the modified electronic structures. This work demonstrates the manipulation of the rich phases and superstructures of monolayer TaTe2 films by controlling the growth kinetics and post-growthannealing.

Chiral Dirac Fermion in a Collinear Antiferromagnet

In a Dirac semimetal, the massless Dirac fermion has zero chirality, leading to surface states connected adiabatically to a topologically trivial surface state as well as vanishing anomalous Hall effect. Recently, it is predicted that in the nonrelativistic limit of certain collinear antiferromagnets, there exists a type of chiral “Dirac-like” fermion, whose dispersion manifests four-fold degenerate crossing points formed by spin-degenerate linear bands, with topologically protected Fermi arcs. Such an unconventional chiral fermion, protected by a hidden SU(2) symmetry in the hierarchy of an enhanced crystallographic group, namely spin space group, is not experimentally verified yet. Here, by angle-resolved photoemission spectroscopy measurements, we reveal the surface origin of the electron pocket at the Fermi surface in collinear antiferromagnet CoNb3S6. Combining with neutron diffraction and first-principles calculations, we suggest a multidomain collinear antiferromagnetic configuration, rendering the the existence of the Fermi-arc surface states induced by chiral Dirac-like fermions. Our work provides spectral evidence of the chiral Dirac-like fermion caused by particular spin symmetry in CoNb3S6, paving an avenue for exploring new emergent phenomena in antiferromagnets with unconventional quasiparticle excitations.

Electronic band structure of superconducting KTaO3 (111) interfaces

Two-dimensional electron gases (2DEGs) based on KTaO3 are emerging as a promising platform for spin-orbitronics due to their high Rashba spin–orbit coupling (SOC) and gate-voltage tunability. The recent discovery of a superconducting state in KTaO3 2DEGs now expands their potential towards topological superconductivity. Although the band structure of KTaO3 surfaces of various crystallographic orientations has already been mapped using angle-resolved photoemission spectroscopy (ARPES), this is not the case for superconducting KTaO3 2DEGs. Here, we reveal the electronic structure of superconducting 2DEGs based on KTaO3 (111) single crystals through ARPES measurements. We fit the data with a tight-binding model and compute the associated spin textures to bring insight into the SOC-driven physics of this fascinating system.

Dirac-fermion-assisted interfacial superconductivity in epitaxial topological-insulator/iron-chalcogenide heterostructures

Over the last decade, the possibility of realizing topological superconductivity (TSC) has generated much excitement. TSC can be created in electronic systems where the topological and superconducting orders coexist, motivating the continued exploration of candidate material platforms to this end. Here, we use molecular beam epitaxy (MBE) to synthesize heterostructures that host emergent interfacial superconductivity when a non-superconducting antiferromagnet (FeTe) is interfaced with a topological insulator (TI) (Bi, Sb)2Te3. By performing in-vacuo angle-resolved photoemission spectroscopy (ARPES) and ex-situ electrical transport measurements, we find that the superconducting transition temperature and the upper critical magnetic field are suppressed when the chemical potential approaches the Dirac point. We provide evidence to show that the observed interfacial superconductivity and its chemical potential dependence is the result of the competition between the Ruderman-Kittel-Kasuya-Yosida-type ferromagnetic coupling mediated by Dirac surface states and antiferromagnetic exchange couplings that generate the bicollinear antiferromagnetic order in the FeTe layer.