High-resolution Angle-resolved Photoemission Spectroscopy Research Articles

Possible spin excitation structure in monolayer FeSe grown on SrTiO3

Based on recent high-resolution angle-resolved photoemission spectroscopy measurement in monolayer FeSe grown on SrTiO$_{3}$, we constructed a tight-binding model and proposed a superconducting (SC) pairing function which can well fit the observed band structure and SC gap anisotropy. Then we investigated the spin excitation spectra in order to determine the possible sign structure of the SC order parameter. We found that a resonance-like spin excitation may occur if the SC order parameter changes sign along the Fermi surfaces. However, this resonance is located at different locations in momentum space compared to other FeSe-based superconductors, suggesting that the Fermi surface shape and pairing symmetry in monolayer FeSe grown on SrTiO$_{3}$ may be different from other FeSe-based superconductors.

Electronic structure of RSb ( R=Y , Ce, Gd, Dy, Ho, Tm, Lu) studied by angle-resolved photoemission spectroscopy

We use high resolution angle-resolved photoemission spectroscopy (ARPES) and electronic structure calculations to study the electronic properties of rare-earth monoantimonides RSb (R = Y, Ce, Gd, Dy, Ho, Tm, Lu). The experimentally measured Fermi surface (FS) of RSb consists of at least two concentric hole pockets at the $\Gamma$ point and two intersecting electron pockets at the $X$ point. These data agree relatively well with the electronic structure calculations. Detailed photon energy dependence measurements using both synchrotron and laser ARPES systems indicate that there is at least one Fermi surface sheet with strong three-dimensionality centered at the $\Gamma$ point. Due to the "lanthanide contraction", the unit cell of different rare-earth monoantimonides shrinks when changing rare-earth ion from CeSb to LuSb. This results in the differences in the chemical potentials in these compounds, which is demonstrated by both ARPES measurements and electronic structure calculations. Interestingly, in CeSb, the intersecting electron pockets at the $X$ point seem to be touching the valence bands, forming a four-fold degenerate Dirac-like feature. On the other hand, the remaining rare-earth monoantimonides show significant gaps between the upper and lower bands at the $X$ point. Furthermore, similar to the previously reported results of LaBi, a Dirac-like structure was observed at the $\Gamma$ point in YSb, CeSb, and GdSb, compounds showing relatively high magnetoresistance. This Dirac-like structure may contribute to the unusually large magnetoresistance in these compounds.

Electronic bandstructure and van der Waals coupling of ReSe2 revealed by high-resolution angle-resolved photoemission spectroscopy

ReSe2 and ReS2 are unusual compounds amongst the layered transition metal dichalcogenides as a result of their low symmetry, with a characteristic in-plane anisotropy due to in-plane rhenium ‘chains’. They preserve inversion symmetry independent of the number of layers and, in contrast to more well-known transition metal dichalcogenides, bulk and few-monolayer Re-TMD compounds have been proposed to behave as electronically and vibrational decoupled layers. Here, we probe for the first time the electronic band structure of bulk ReSe2 by direct nanoscale angle-resolved photoemission spectroscopy. We find a highly anisotropic in- and out-of-plane electronic structure, with the valence band maxima located away from any particular high-symmetry direction. The effective mass doubles its value perpendicular to the Re chains and the interlayer van der Waals coupling generates significant electronic dispersion normal to the layers. Our density functional theory calculations, including spin-orbit effects, are in excellent agreement with these experimental findings.

Direct observation of how the heavy-fermion state develops in CeCoIn5

Heavy fermion materials gain high electronic masses and expand Fermi surfaces when the high-temperature localized f electrons become itinerant and hybridize with the conduction band at low temperatures. However, despite the common application of this model, direct microscopic verification remains lacking. Here we report high-resolution angle-resolved photoemission spectroscopy measurements on CeCoIn5, a prototypical heavy fermion compound, and reveal the long-sought band hybridization and Fermi surface expansion. Unexpectedly, the localized-to-itinerant transition occurs at surprisingly high temperatures, yet f electrons are still largely localized at the lowest temperature. Moreover, crystal field excitations likely play an important role in the anomalous temperature dependence. Our results paint an comprehensive unanticipated experimental picture of the heavy fermion formation in a periodic multi-level Anderson/Kondo lattice, and set the stage for understanding the emergent properties in related materials.

Rotatable high-resolution ARPES system for tunable linear-polarization geometry

A rotatable high-resolution angle-resolved photoemission spectroscopy (ARPES) system has been developed to utilize tunable linear-polarization geometries on the linear undulator beamline (BL-1) at Hiroshima Synchrotron Radiation Center. By rotating the whole ARPES measurement system, the photoelectron detection plane can be continuously changed from parallel to normal against the electric field vector of linearly polarized undulator radiation. This polarization tunability enables us to identify the symmetry of the initial electronic states with respect to the mirror planes, and to selectively observe the electronic states based on the dipole selection rule in the photoemission process. Specifications of the rotatable high-resolution ARPES system are described, as well as its capabilities with some representative experimental results.

Dimensional Crossover in a Charge Density Wave Material Probed by Angle-Resolved Photoemission Spectroscopy.

High-resolution angle-resolved photoemission spectroscopy data reveal evidence of a crossover from one-dimensional (1D) to three-dimensional (3D) behavior in the prototypical charge density wave (CDW) material NbSe_{3}. In the low-temperature 3D regime, gaps in the electronic structure are observed due to two incommensurate CDWs, in agreement with x-ray diffraction and electronic-structure calculations. At higher temperatures we observe a spectral weight depletion that approaches the power-law behavior expected in one dimension. From the warping of the quasi-1D Fermi surface at low temperatures, we extract the energy scale of the dimensional crossover. This is corroborated by a detailed analysis of the density of states, which reveals a change in dimensional behavior dependent on binding energy. Our results offer an important insight into the dimensionality of excitations in quasi-1D materials.

Electronic structure of FeS

Here we report the electronic structure of FeS, a recently identified iron-based superconductor. Our high-resolution angle-resolved photoemission spectroscopy studies show two hole-like ($\alpha$ and $\beta$) and two electron-like ($\eta$ and $\delta$) Fermi pockets around the Brillouin zone center and corner, respectively, all of which exhibit moderate dispersion along $k_z$. However, a third hole-like band ($\gamma$) is not observed, which is expected around the zone center from band calculations and is common in iron-based superconductors. Since this band has the highest renormalization factor and is known to be the most vulnerable to defects, its absence in our data is likely due to defect scattering --- and yet superconductivity can exist without coherent quasiparticles in the $\gamma$ band. This may help resolve the current controversy on the superconducting gap structure of FeS. Moreover, by comparing the $\beta$ bandwidths of various iron chalcogenides, including FeS, FeSe$_{1-x}$S$_x$, FeSe, and FeSe$_{1-x}$ Te$_x$, we find that the $\beta$ bandwidth of FeS is the broadest. However, the band renormalization factor of FeS is still quite large, when compared with the band calculations, which indicates sizable electron correlations. This explains why the unconventional superconductivity can persist over such a broad range of isovalent substitution in FeSe$_{1-x}$Te$_{x}$ and FeSe$_{1-x}$S$_{x}$.

Strongly enhanced temperature dependence of the chemical potential in FeSe

Employing a 10-orbital tight binding model, we present a new set of hopping parameters fitted directly to our latest high resolution angle-resolved photoemission spectroscopy (ARPES) data for the high temperature tetragonal phase of FeSe. Using these parameters we predict a large 10 meV shift of the chemical potential as a function of temperature. In order to confirm this large temperature dependence, we performed ARPES experiments on FeSe and observed a $\sim$25 meV rigid shift to the chemical potential between 100 K and 300 K. This unexpectedly strong shift has important implications for theoretical models of superconductivity and of nematic order in FeSe materials.

Band splitting and Weyl nodes in trigonal tellurium studied by angle-resolved photoemission spectroscopy and density functional theory

We have performed high-resolution angle-resolved photoemission spectroscopy (ARPES) on trigonal tellurium consisting of helical chains in the crystal. Through the band-structure mapping in the three-dimensional Brillouin zone, we found a definitive evidence for the band splitting originating from the chiral nature of crystal. A direct comparison of the band dispersion between the ARPES results and the first-principles band-structure calculations suggests the presence of Weyl nodes and tiny spin-polarized hole pockets around the H point. The present result opens a pathway toward studying the interplay among crystal symmetry, band structure, and exotic physical properties in chiral crystals.

Compelling experimental evidence of a Dirac cone in the electronic structure of a 2D Silicon layer

The remarkable properties of graphene stem from its two-dimensional (2D) structure, with a linear dispersion of the electronic states at the corners of the Brillouin zone (BZ) forming a Dirac cone. Since then, other 2D materials have been suggested based on boron, silicon, germanium, phosphorus, tin, and metal di-chalcogenides. Here, we present an experimental investigation of a single silicon layer on Au(111) using low energy electron diffraction (LEED), high resolution angle-resolved photoemission spectroscopy (HR-ARPES), and scanning tunneling microscopy (STM). The HR-ARPES data show compelling evidence that the silicon based 2D overlayer is responsible for the observed linear dispersed feature in the valence band, with a Fermi velocity of comparable to that of graphene. The STM images show extended and homogeneous domains, offering a viable route to the fabrication of silicene-based opto-electronic devices.

Shifts and Splittings of the Hole Bands in the Nematic Phase of FeSe

We report a high-resolution laser-based angle-resolved photoemission spectroscopy (laser-ARPES) study of single crystals of FeSe, focusing on the temperature-dependence of the hole-like bands around the ${\rm \Gamma}$ point. As the system cools through the tetragonal-orthorhombic "nematic" structural transition at 90~K, the splitting of the $d_{xz}$/$d_{yz}$ bands is observed to increase by a magnitude of 13 meV. Moreover, the onset of a $\sim$10 meV downward shift of the $d_{xy}$ band is also at 90~K. These measurements provide clarity on the nature, magnitude and temperature-dependence of the band shifts at the ${\rm \Gamma}$ point in the nematic phase of FeSe.

Direct observation of the band structure in bulk hexagonal boron nitride

A promising route towards nanodevice applications relies on the association of graphene and transition metal dichalcogenides with hexagonal boron nitride (h-BN). Due to its insulating nature, h-BN has emerged as a natural substrate and gate dielectric for graphene-based electronic devices. However, some fundamental properties of bulk h-BN remain obscure. For example, the band structure and the position of the Fermi level have not been experimentally resolved. Here, we report a direct observation of parabolic dispersions of h-BN crystals using high-resolution angle-resolved photoemission spectroscopy (ARPES). We find that h-BN exfoliation on epitaxial graphene enables overcoming the technical difficulties of using ARPES with insulating materials. We show trigonal warping of the intensity maps at constant energy. The valence-band maxima are located around the K points, 2.5 eV below the Fermi level, thus confirming the residual p-type character of typical h-BN.

Bulk and surface electronic structure of hexagonal structuredPtBi2studied by angle-resolved photoemission spectroscopy

PtBi2 with a layered trigonal crystal structure was recently reported to exhibit an unconventional large linear magnetoresistance, while the mechanism involved is still elusive. Using high resolution angle-resolved photoemission spectroscopy, we present a systematic study on its bulk and surface electronic structure. Through careful comparison with first-principle calculations, our experiment distinguishes the low-lying bulk bands from entangled surface states, allowing the estimation of the real stoichiometry of samples. We find significant electron doping in PtBi2, implying a substantial Bi deficiency induced disorder therein. We discover a Dirac-cone-like surface state on the boundary of the Brillouin zone, which is identified as an accidental Dirac band without topological protection. Our findings exclude quantum-limit-induced linear band dispersion as the cause of the unconventional large linear magnetoresistance.

Evidence for unidirectional nematic bond ordering in FeSe

The lifting of $d_{xz}$-$d_{yz}$ orbital degeneracy is often considered a hallmark of the nematic phase of Fe-based superconductors, including FeSe, but its origin is not yet understood. Here we report a high resolution Angle-Resolved Photoemission Spectroscopy study of single crystals of FeSe, accounting for the photon-energy dependence and making a detailed analysis of the temperature dependence. We find that the hole pocket undergoes a fourfold-symmetry-breaking distortion in the nematic phase below 90~K, but in contrast the changes to the electron pockets do not require fourfold symmetry-breaking. Instead, there is an additional separation of the existing $d_{xy}$ and $d_{xz/yz}$ bands - which themselves are not split within resolution. These observations lead us to propose a new scenario of "unidirectional nematic bond ordering" to describe the low-temperature electronic structure of FeSe, supported by a good agreement with 10-orbital tight binding model calculations.

Observation of the spin-polarized surface state in a noncentrosymmetric superconductor BiPd.

Recently, noncentrosymmetric superconductor BiPd has attracted considerable research interest due to the possibility of hosting topological superconductivity. Here we report a systematic high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES study of the normal state electronic and spin properties of BiPd. Our experimental results show the presence of a surface state at higher-binding energy with the location of Dirac point at around 700 meV below the Fermi level. The detailed photon energy, temperature-dependent and spin-resolved ARPES measurements complemented by our first-principles calculations demonstrate the existence of the spin-polarized surface states at high-binding energy. The absence of such spin-polarized surface states near the Fermi level negates the possibility of a topological superconducting behaviour on the surface. Our direct experimental observation of spin-polarized surface states in BiPd provides critical information that will guide the future search for topological superconductivity in noncentrosymmetric materials.

Unconventional electronic structure of silicene on Ag/H-Si(111)

We fabricated monolayer silicene on a thin silver (Ag) crystal film grown on hydrogen-terminated Si(111), and studied the crystal and the electronic structure by low-energy electron diffraction (LEED) and high-resolution angle-resolved photoemission spectroscopy (ARPES). The fabricated sample exhibits the 3×3 LEED pattern characteristic of silicene and the band dispersions with the periodicity of the silicene Brillouin zone, indicative of successful fabrication of silicene on Ag/H-Si(111). However, we observed no signature for the Dirac-cone state at the K point, while the observed band structure exhibits an unexpected van-Hove singularity with a saddle point at the binding energy of 1eV. Such a singularity has not been reproduced in so-far existing band structure calculations, requesting sophisticated calculations incorporating the complicated strong hybridization between silicene and Ag orbitals.

Band structure characterization of WS2 grown by chemical vapor deposition

Growth by chemical vapor deposition (CVD) leads to multilayer WS2 of very high quality, based on high-resolution angle-resolved photoemission spectroscopy. The experimental valence band electronic structure is considered to be in good agreement with that obtained from density functional theory calculations. We find the spin-orbit splitting at the K¯ point to be 420 ± 20 meV with a hole effective mass of −0.35 ± 0.02 me for the upper spin-orbit component (the branch closer to the Fermi level) and −0.43 ± 0.07 me for the lower spin-orbit component. As predicted by theory, a thickness-dependent increase of bandwidth is observed at the top of the valence band, in the region of the Brillouin zone center. The top of the valence band of the CVD-prepared films exhibits a substantial binding energy, consistent with n-type behavior, and in agreement with transistor characteristics acquired using devices incorporating the same WS2 material.

Observation of metallic surface states in the strongly correlated Kitaev-Heisenberg candidateNa2IrO3

We report high-resolution angle-resolved photoemission spectroscopy measurements on the honeycomb iridate Na2IrO3. Our measurements reveal the existence of a metallic surface band feature crossing the Fermi level with nearly linear dispersion and an estimated surface carrier density of 3.2 $\times$ 10$^{13}$ cm$^{-2}$, which has not been theoretically predicted or experimentally observed, and provides the first evidence for metallic behavior on the boundary of this material, whereas the bulk bands exhibit a robust insulating gap. We further show the lack of theoretically predicted Dirac cones at the $\overline{M}$ points of the surface Brillouin zone, which confirms the absence of a stacked quantum spin Hall phase in this material. Our data indicates that the surface ground state of this material is exotic and metallic, unlike as predicted in theory, and establishes Na2IrO3 as a rare example of a strongly correlated spin-orbit insulator with surface metallicity.

Enhancement of electron–phonon coupling in Cs-overlayered intercalated bilayer graphene

We have performed high-resolution angle-resolved photoemission spectroscopy (ARPES) on cesium (Cs) intercalated bilayer graphene with a Cs overlayer (Cs-C8CsC8). Low-energy electron diffraction shows a (2 × 2) pattern consistent with intercalation of a Cs layer similar to bulk C8Cs, in addition to the signature of a nearly commensurate superstructure created by the Cs overlayer. ARPES results reveal folding of the π bands due to the periodic (2 × 2) potential of the intercalated Cs atoms, together with a free-electron-like state at the point. Significant mass renormalization is observed in the band dispersion near the Fermi level, indicative of strong electron–phonon coupling. Based on analysis of the self-energy, we find anisotropic electron–phonon coupling with an estimated strength of ± 0.02 in the K- direction, and in the K-M direction. This coupling is much larger than that of other doped graphenes, and comparable to superconducting bulk GICs. We attribute this large electron–phonon coupling constant to the presence of the Cs overlayer, which highly dopes bands, and creates a structure similar to stage-I graphite intercalation compounds.

Direct observation of nonequivalent Fermi-arc states of opposite surfaces in the noncentrosymmetric Weyl semimetal NbP

We have performed high-resolution angle-resolved photoemission spectroscopy (ARPES) on noncentrosymmetric Weyl semimetal candidate NbP, and determined the electronic states of both Nb- and P-terminated surfaces corresponding to the "opposite" surfaces of a polar crystal. We revealed a drastic difference in the Fermi-surface topology between the opposite surfaces, whereas the Fermi arcs on both surfaces are likely terminated at the surface projection of the same bulk Weyl nodes. Comparison of the ARPES data with our first-principles band calculations suggests notable difference in electronic structure at the Nb-terminated surface between theory and experiment. The present result opens a platform for realizing exotic quantum phenomena arising from unusual surface properties of Weyl semimetals.