Search Results (36)

Occupied and unoccupied electronic states of altermagnetic MnTe(0001) single crystals were studied by photoemission and inverse-photoemission spectroscopies after establishing a reproducible surface cleaning procedure involving repeated sputtering and annealing cycles. The angle-resolved photoemission spectroscopy (ARPES) exhibited a hole-like band dispersion centered at the $\overline{\mathsf{\Gamma }}$ point, which was consistent with the reported ARPES results and our density functional theory (DFT) calculations with the on-site Coulomb interaction U. The observed Mn 3d↑-derived peak at −3.5 eV, however, significantly deviated from the DFT + U calculations. Meanwhile, the Mn 3d↓-derived peak at +3.0 eV observed by inverse-photoemission spectroscopy agreed well with the DFT + U results. Based on simulations of the spectral function employing an w-dependent model self-energy, we found significant relaxation effects in the electron-removal process, while such effects were negligible in the electron-addition process. Our study provides a comprehensive picture of electronic states, forming a solid foundation for understanding the magnetic and transport properties of MnTe. Full article

SnSe₂, as a prominent member of the post-transition metal dichalcogenides, exhibits many intriguing physical phenomena and excellent thermoelectric properties, calling for both fundamental study and potential application in two-dimensional (2D) devices. In this article, we realized the molecular beam epitaxial growth of SnSe₂ films on a $\sqrt{3}\times \sqrt{3}$-Sn reconstructed Si(111) surface. The analysis of reflection high-energy electron diffraction reveals the in-plane lattice orientation as SnSe₂[110]//$\sqrt{3}$-Sn [112]//Si [110]. In addition, the flat morphology of SnSe₂ film was identified by scanning tunneling microscopy (STM), implying the relatively strong adsorption effect of $\sqrt{3}$-Sn/Si(111) substrate to the SnSe₂ adsorbates. Subsequently, the interfacial charge transfer was observed by X-ray photoemission spectroscopy. Afterwards, the direct characterization of electronic structures was obtained via angle-resolved photoemission spectroscopy. In addition to proving the presence of interfacial charge transfer again, a new relatively flat in-gap band was found in monolayer and few-layer SnSe₂, which disappeared in multi-layer SnSe₂. The interface strain-induced partial structural phase transition of thin SnSe₂ films is presumed to be the reason. Our results provide important information on the characterization and effective modulation of electronic structures of SnSe₂ grown on $\sqrt{3}$-Sn/Si(111), paving the way for the further study and application of SnSe₂ in 2D electronic devices. Full article

The family of BiS₂-based superconductors has attracted considerable attention since their discovery in 2012 due to the unique structural and electronic properties of these materials. Several experimental and theoretical studies have been performed to explore the basic properties and the underlying mechanism for superconductivity. In this review, we discuss the current understanding of pairing symmetry in BiS₂-based superconductors and particularly the role of point-contact spectroscopy in unravelling the mechanism underlying the superconducting state. We also review experimental results obtained with different techniques including angle-resolved photoemission spectroscopy, scanning tunnelling spectroscopy, specific heat measurements, and nuclear magnetic resonance spectroscopy. The integration of experimental results and theoretical predictions sheds light on the complex interplay between electronic correlations, spin fluctuations, and Fermi surface topology in determining the coupling mechanism. Finally, we highlight recent advances and future directions in the field of BiS₂-based superconductors, underlining the potential technological applications. Full article

For more than a decade, the unusual distribution of electrons observed in ARPES (angle-resolved photoemission spectroscopy) data within the energy range of ~30 meV to ~300 meV below the Fermi level, known as the ARPES energy range, has remained a puzzle in the field of iron-based superconductivity. As the electron–phonon coupling of FeSe/SrTiO₃ is very strong, our investigation is centered on exploring the synergistic interplay between spin-density waves (SDW) and charge-density waves (CDW) with differential phonons at the interface between antiferromagnetic maxima and minima under wave interference. Our analysis reveals that the synergistic energy is proportional to the ARPES energy range, as seen in the comparison between FeSe and FeSe/SrTiO₃. This finding may suggest that the instantaneous interplay between these intricate phenomena may play a role in triggering the observed energy range in ARPES. Full article

Here, by using angle-resolved photoemission spectroscopy, we showed that Bi_2−xCr_xSe₃ single crystals have a distinctly well-defined band structure with a large bulk band gap and undistorted topological surface states. These spectral features are unlike their thin film forms in which a large nonmagnetic gap with a distorted band structure was reported. We further provide laser-based high resolution photoemission data which reveal a Dirac point gap even in the pristine sample. The gap becomes more pronounced with Cr doping into the bulk of Bi₂Se₃. These observations show that the Dirac point can be modified by the magnetic impurities as well as the light source. Full article

Periodic lattice distortion, known as the charge density wave, is generally attributed to electron–phonon coupling. This correlation is expected to induce a pseudogap at the Fermi level in order to gain the required energy for stable lattice distortion. The transition metal dichalcogenide 1T-VSe₂ also undergoes such a transition at 110 K. Here, we present detailed angle-resolved photoemission spectroscopy experiments to investigate the electronic structure in 1T-VSe₂ across the structural transition. Previously reported warping of the electronic structure and the energy shift of a secondary peak near the Fermi level as the origin of the charge density wave phase are shown to be temperature independent and hence cannot be attributed to the structural transition. Our work reveals new states that were not resolved in previous studies. Earlier results can be explained by the different dispersion natures of these states and temperature-induced broadening. Only the overall size of the Fermi surface is found to change across the structural transition. These observations, quite different from the charge density wave scenario commonly considered for 1T-VSe₂ and other transition metal dichalcogenides, bring fresh perspectives toward correctly describing structural transitions. Therefore, these new results can be applied to material families in which the origin of the structural transition has not been resolved. Full article

Over the last two decades, time- and angle-resolved photoemission spectroscopy (trARPES) has become a mature and established experimental technique for the study of ultrafast electronic and structural dynamics in materials. To date, most trARPES investigations have focused on the investigation of processes occurring on time scales of ≳30 fs, in particular, relaxation and thermalization, and have therefore been blind to the initial sub-10 fs dynamics related to electronic coherence and correlation effects. In this article, we illustrate how current trARPES setups reach their limits when it comes to addressing such extraordinarily short time scales and present an experimental configuration that provides the time, energy, and momentum resolutions required to monitor few-femtosecond dynamics on the relevant energy and momentum scales. We discuss the potential capabilities of such an experiment to study the electronic response of materials in the strong-field interaction regime at PHz frequencies and finally review a theoretical concept that may in the future even overcome the competing resolution limitations of trARPES experiments, as imposed by the time–bandwidth product of the probing laser pulse. Our roadmap for ultrafast trARPES indicates a path to break new experimental ground in quantum nonequilibrium electronic dynamics, from which new possibilities for ultrafast control of optical and electronic signals in quantum materials can be explored. Full article

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. Full article

One of the approaches to manipulate MnBi${}_2$Te${}_4$ properties is the magnetic dilution, which inevitably affects the interplay of magnetism and band topology in the system. In this work, we carried out angle-resolved photoemission spectroscopy (ARPES) measurements and density functional theory (DFT) calculations for analysing changes in the electronic structure of Mn${}_{1-x}$Ge${}_x$Bi${}_2$Te${}_4$ that occur under parameter x variation. We consider two ways of Mn/Ge substitution: (i) bulk doping of the whole system; (ii) surface doping of the first septuple layer. For the case (i), the experimental results reveal a decrease in the value of the bulk band gap, which should be reversed by an increase when the Ge concentration reaches a certain value. Ab-initio calculations show that at Ge concentrations above 50%, there is an absence of the bulk band inversion of the Te $p_z$ and Bi $p_z$ contributions at the $\Gamma$-point with significant spatial redistribution of the states at the band gap edges into the bulk, suggesting topological phase transition in the system. For case (ii) of the vertical heterostructure Mn${}_{1-x}$Ge${}_x$Bi${}_2$Te${}_4$/MnBi${}_2$Te${}_4$, it was shown that an increase of Ge concentration in the first septuple layer leads to effective modulation of the Dirac gap in the absence of significant topological surface states of spatial redistribution. The results obtained indicate that surface doping compares favorably compared to bulk doping as a method for the Dirac gap value modulation. Full article

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. Full article

First-principles calculations for underdoped La_2−xSr_xCuO₄ (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 T_c(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 T_c. We also show that the relationship T*(x_c) = T_c(x_c) holds at x_c = 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. Full article

Scientific data acquisition is a problem domain that has been underserved by its computational tools despite the need to efficiently use hardware, to guarantee validity of the recorded data, and to rapidly test ideas by configuring experiments quickly and inexpensively. High-dimensional physical spectroscopies, such as angle-resolved photoemission spectroscopy, make these issues especially apparent because, while they use expensive instruments to record large data volumes, they require very little acquisition planning. The burden of writing data acquisition software falls to scientists, who are not typically trained to write maintainable software. In this paper, we introduce AutodiDAQt to address these shortfalls in the scientific ecosystem. To ground the discussion, we demonstrate its merits for angle-resolved photoemission spectroscopy and high bandwidth spectroscopies. AutodiDAQt addresses the essential needs for scientific data acquisition by providing simple concurrency, reproducibility, retrospection of the acquisition sequence, and automated user interface generation. Finally, we discuss how AutodiDAQt enables a future of highly efficient machine-learning-in-the-loop experiments and analysis-driven experiments without requiring data acquisition domain expertise by using analysis code for external data acquisition planning. Full article

Porous transition metal oxides are widely studied as biocompatible materials for the development of prosthetic implants. Resurfacing the oxide to improve the antibacterial properties of the material is still an open issue, as infections remain a major cause of implant failure. We investigated the functionalization of porous titanium oxide obtained by anodic oxidation with amino acids (Leucine) as a first step to couple antimicrobial peptides to the oxide surface. We adopted a two-step molecular deposition process as follows: self-assembly of aminophosphonates to titanium oxide followed by covalent coupling of Fmoc-Leucine to aminophosphonates. Molecular deposition was investigated step-by-step by Atomic Force Microscopy (AFM) and X-ray Photoemission Spectroscopy (XPS). Since the inherent high roughness of porous titanium hampers the analysis of molecular orientation on the surface, we resorted to parallel experiments on flat titanium oxide thin films. AFM nanoshaving experiments on aminophosphonates deposited on flat TiO₂ indicate the formation of an aminophosphonate monolayer while angle-resolved XPS analysis gives evidence of the formation of an oriented monolayer exposing the amine groups. The availability of the amine groups at the outer interface of the monolayer was confirmed on both flat and porous substrates by the following successful coupling with Fmoc-Leucine, as indicated by high-resolution XPS analysis. Full article

The discovery of high-$T_c$ superconductivity in cuprates in 1986 moved strongly correlated systems from exotic worlds interesting only for pure theorists to the focus of solid-state research. In recent decades, the majority of hot topics in condensed matter physics (high-$T_c$ superconductivity, colossal magnetoresistance, multiferroicity, ferromagnetism in diluted magnetic semiconductors, etc.) have been related to strongly correlated transition metal compounds. The highly successful electronic structure calculations based on density functional theory lose their predictive power when applied to such compounds. It is necessary to go beyond the mean field approximation and use the many-body theory. The methods and models that were developed for the description of strongly correlated systems are reviewed together with the examples of response function calculations that are needed for the interpretation of experimental information (inelastic neutron scattering, optical conductivity, resonant inelastic X-ray scattering, electron energy loss spectroscopy, angle-resolved photoemission, electron spin resonance, and magnetic and magnetoelectric properties). The peculiarities of (quasi-) 0-, 1-, 2-, and 3- dimensional systems are discussed. Full article

Mg₃Sb₂-based compounds are one type of important room-temperature thermoelectric materials and the appropriate candidate of type-II nodal line semimetals. In Mg₃Sb₂-based films, compelling research topics such as dimensionality reduction and topological states rely on the controllable preparation of films with high crystallinity, which remains a big challenge. In this work, high quality Mg₃Sb₂ films are successfully grown on mismatched substrates of sapphire (000l), while the temperature-driven twin structure evolution and characteristics of the electronic structure are revealed in the as-grown Mg₃Sb₂ films by in situ and ex situ measurements. The transition of layer-to-island growth of Mg₃Sb₂ films is kinetically controlled by increasing the substrate temperature (T_sub), which is accompanied with the rational manipulation of twin structure and epitaxial strains. Twin-free structure could be acquired in the Mg₃Sb₂ film grown at a low T_sub of 573 K, while the formation of twin structure is significantly promoted by elevating the T_sub and annealing, in close relation to the processes of strain relaxation and enhanced mass transfer. Measurements of scanning tunneling spectroscopy (STS) and angle-resolved photoemission spectroscopy (ARPES) elucidate the intrinsic p-type conduction of Mg₃Sb₂ films and a bulk band gap of ~0.89 eV, and a prominent Fermi level downshift of ~0.2 eV could be achieved by controlling the film growth parameters. As elucidated in this work, the effective manipulation of the epitaxial strains, twin structure and Fermi level is instructive and beneficial for the further exploration and optimization of thermoelectric and topological properties of Mg₃Sb₂-based films. Full article