Angle-resolved Photoemission Data Research Articles

A minimalist approach to 3D photoemission orbital tomography: algorithms and data requirements

Photoemission orbital tomography provides direct access from laboratory measurements to the real-space molecular orbitals of well-ordered organic semiconductor layers. Specifically, the application of phase retrieval algorithms to photon-energy- and angle-resolved photoemission data enables the direct reconstruction of full 3D molecular orbitals without the need for simulations using density functional theory or the like. However, until now this procedure has remained challenging due to the need for densely-sampled, well-calibrated 3D photoemission patterns. Here, we present an iterative projection algorithm that completely eliminates this challenge: for the benchmark case of the pentacene frontier orbitals, we demonstrate the reconstruction of the full orbital based on a dataset containing only four simulated photoemission momentum measurements. We discuss the algorithm performance, sampling requirements with respect to the photon energy, optimal measurement strategies, and the accuracy of orbital images that can be achieved.

Fate of Quasiparticles at High Temperature in the Correlated Metal Sr_{2}RuO_{4}.

We study the temperature evolution of quasiparticles in the correlated metal Sr_{2}RuO_{4}. Our angle resolved photoemission data show that quasiparticles persist up to temperatures above 200K, far beyond the Fermi liquid regime. Extracting the quasiparticle self-energy, we demonstrate that the quasiparticle residue Z increases with increasing temperature. Quasiparticles eventually disappear on approaching the bad metal state of Sr_{2}RuO_{4} not by losing weight but via excessive broadening from super-Planckian scattering. We further show that the Fermi surface of Sr_{2}RuO_{4}-defined as the loci where the spectral function peaks-deflates with increasing temperature. These findings are in semiquantitative agreement with dynamical mean field theory calculations.

Paramagnetic electronic structure of CrSBr: Comparison between ab initio GW theory and angle-resolved photoemission spectroscopy

We explore the electronic structure of paramagnetic CrSBr by comparative first principles calculations and angle-resolved photoemission spectroscopy. We theoretically approximate the paramagnetic phase using a supercell hosting spin configurations with broken long-range order and applying quasiparticle self-consistent $GW$ theory, without and with the inclusion of excitonic vertex corrections to the screened Coulomb interaction (QS$GW$ and QS$G\hat{W}$, respectively). Comparing the quasi-particle band structure calculations to angle-resolved photoemission data collected at 200 K results in excellent agreement. This allows us to qualitatively explain the significant broadening of some bands as arising from the broken magnetic long-range order and/or electronic dispersion perpendicular to the quasi two-dimensional layers of the crystal structure. The experimental band gap at 200 K is found to be at least 1.51 eV at 200 K. At lower temperature, no photoemission data can be collected as a result of charging effects, pointing towards a significantly larger gap, which is consistent with the calculated band gap of $\approx$ 2.1 eV.

Theory of circular dichroism in angle-resolved resonant photoemission from magnetic surfaces

A theoretical method is presented for angle-resolved photoemission at the transition metal $L$-edge resonance. It combines atomic multiplet calculations for the second-order resonant photoemission amplitude on the core-level site and a single scattering calculation of the photoelectron final state. The theory is applied to a magnetized Ni(111) surface excited with circularly polarized x rays at the Ni ${L}_{2,3}$-edge resonance with a focus on the circular dichroism (CD) signal. Good agreement with available experimental data is achieved. It is shown that the CD pattern is composed of a slowly varying magnetic signal induced by the atomic resonant process and a signal of fast angular modulations that are due to the interference of primary and scattered waves, known as the Daimon effect. The two types of CD signals are found to be nearly additive. At the Ni ${L}_{2}$-edge resonance, the angular dependence of the magnetic CD is well described by a simple expression known from x-ray magnetic CD. At the ${L}_{3}$ edge, however, the angular dependence is more complex and shows a pronounced final state multiplet dependence. With the present theory, it becomes possible to extract element- and site-selective magnetic information of surfaces from the CD in angle-resolved resonant photoemission data.

Mott physics: One of main themes in quantum materials

<sec>The competition and cooperation between the itinerancy behavior and localization behavior of electrons in correlated quantum materials, known as Mott physics, is the physical mechanism behind the diverse states of many quantum materials. This article reviews the manifestation of Mott physics in various quantum materials and establishes it as one of the main themes of quantum materials. Finding and understanding its ever-changing ways of manifestation is one of the central tasks of experimental research on condensed matter physics.</sec><sec>Specifically, the filling-control route of Mott transition is illustrated by exampling the surface K-dosed Sr<sub>2</sub>IrO<sub>4</sub>, which exhibits d-wave gap, pseudogap behavior in underdoped regime, and phase separation with inhomogeneous electronic state distribution. All of these show strong resemblances to the doped cuprate superconductors, another prototypical filling-control type of Mott transition case. On the other hand, the bandwidth-control route of Mott transition could be found in NiS<sub>2–<i>x</i></sub>Se<sub><i>x</i></sub>, where its bandwidth continuously decreases with decreasing Se concentration, until it becomes an insulator. In addition, the essence of various ways of doping in iron-based superconductors is to change their bandwidths. The superconductivity shows up at intermediate bandwidth with moderate correlations, and it diminishes when the bandwidth is large and the electron correlations are weak. For heavily electron-doped iron-selenides, there is even a Mott insulator phase with strong correlations.</sec><sec>For carbon based materials, the phase transition between the antiferromagnetic insulator and superconducting state of A15 Cs<sub>3</sub>C<sub>60</sub> as the volume of fullerene anions decreases could be understood in terms of a bandwidth-control Mott transition; the insulator-superconductor transition discovered in electrically gated “magic angle” twisted-angle bilayer graphene could be understood as a filling-control Mott transition.</sec><sec>For f electron systems, the interplay between itinerancy and localization dominates the heavy fermion behavior and their ground states. The behaviors of the f electrons are demonstrated by using the angle-resolved photoemission data of CeCoIn<sub>5</sub>, whose f electron band becomes more coherent with decreasing temperature, and the c-f hybridization is thus enhanced and the band mass of conduction band continuously increases. The c-f hybridization behaviors of CeCoIn<sub>5,</sub> CeIrIn<sub>5</sub>, and CeRhIn<sub>5</sub> are compared with each other, and the differences in hybridization strength put their ground states into different regimes of the Doniach phase diagram. Similarly, the Skutterudites 4f<sup>2</sup> Kondo lattice system PrOs<sub>4</sub>Sb<sub>12</sub> and its sibling 4f<sup>1</sup> system CeOs<sub>4</sub>Sb<sub>12</sub> also have different ground states due to a slight difference in their c-f hybridization strengths.</sec>

Growth and characterization of high-quality single-crystalline SnTe retaining cubic symmetry down to the lowest temperature studied

SnTe, an archetypical topological crystalline insulator, often shows a transition from a highly symmetric cubic phase to a rhombohedral structure at low temperatures. In order to achieve the cubic phase at low temperatures, we have grown SnTe employing the modified Bridgman method and studied its properties in detail. Analysis of the crystal structure using Laue diffraction and rocking curve measurements shows a high degree of single crystallinity and mosaicity of the sample. The magnetic susceptibility shows diamagnetic behavior, and the specific heat data match phonon contributions typical of a bulk insulator. Resistivity data exhibit metallic conduction similar to two-dimensional systems, and the signature of the structural transition has not been observed down to the lowest temperature studied. Detailed powder x-ray diffraction measurements show a cubic structure in the entire temperature range studied. This is supported by the angle-resolved photoemission data at low temperatures exhibiting a Dirac cone typical of a topological material. These results demonstrate that the ground state structure of SnTe can be stabilized in the cubic phase, providing a promising platform for quantum applications.

Aspects of the normal state resistivity of cuprate superconductors

Planar normal state resistivity data taken from three families of cuprate superconductors are compared with theoretical calculations from the recent extremely correlated Fermi liquid theory (ECFL). The two hole doped cuprate materials $LSCO$ and $BSLCO$ and the electron doped material $LCCO$ have yielded rich data sets at several densities $\delta$ and temperatures T, thereby enabling a systematic comparison with theory. The recent ECFL resistivity calculations for the highly correlated $t$-$t'$-$J$ model by us give the resistivity for a wide set of model parameters. After using X-ray diffraction and angle resolved photoemission data to fix parameters appearing in the theoretical resistivity, only one parameter, the magnitude of the hopping $t$, remains undetermined. For each data set, the slope of the experimental resistivity at a single temperature-density point is sufficient to determine $t$, and hence the resistivity on absolute scale at all remaining densities and temperatures. This procedure is shown to give a fair account of the entire data.

Consistency between ARPES and STM measurements on SmB6

Strongly correlated topological surface states are promising platforms for next-generation quantum applications, but they remain elusive in real materials. The correlated Kondo insulator SmB$_6$ is one of the most promising candidates, with theoretically predicted heavy Dirac surface states supported by transport and scanning tunneling microscopy (STM) experiments. However, a puzzling discrepancy appears between STM and angle-resolved photoemission (ARPES) experiments on SmB$_6$. Although ARPES detects spin-textured surface states, their velocity is an order of magnitude higher than expected, while the Dirac point -- the hallmark of any topological system -- can only be inferred deep within the bulk valence band. A significant challenge is that SmB$_6$ lacks a natural cleavage plane, resulting in ordered surface domains limited to 10s of nanometers. Here we use STM to show that surface band bending can shift energy features by 10s of meV between domains. Starting from our STM spectra, we simulate the full spectral function as an average over multiple domains with different surface potentials. Our simulation shows excellent agreement with ARPES data, and thus resolves the apparent discrepancy between large-area measurements that average over multiple band-shifted domains and atomically-resolved measurements within a single domain.

Electron-phonon coupling in the ordered phase of Rb on monolayer graphene

In the mechanism of two-dimensional (2D) superconductivity in doped graphene, it was predicted that the presence of dopant bands plays a key role. However, it has been challenging to fabricate an ordered phase of alkali metals on graphene owing to its van-der-Waals nature. We systematically study the phase formation of Rb on graphene epitaxially grown on H-passivated SiC(0001). We found a range of control parameters that stabilize the well-ordered 2 × 2 phase (RbC8), as confirmed by in-situ low-energy electron diffraction. Angle-resolved photoemission (ARPES) spectra taken from the 2 × 2 phase show a folded band of graphene and a parabolic band of Rb. In the vicinity of the Fermi level, the self-energy extracted from ARPES data reveals a clear signature of electronic coupling to the in-plane and out-of-plane phonon modes of C and Rb atoms. The electronic coupling of graphene to the in-plane vibration mode of Rb atoms is identified as a key factor for the enhancement of electron-phonon coupling.

Direct hybridization gap from intersite and onsite electronic interactions in CeAg2Ge2.

Electronic and crystal structure studies are presented to describe the role of intersite and onsite interactions for antiferromagnetic ordering in CeAg2Ge2. The crystal structure showed a prominent magnetovolume effect with anomalous negative thermal expansion at low temperature as a consequence of itinerant electron magnetism. The direct hybridization gap with a V-shaped band observed in the angle resolved photoemission data at room temperature, indicates that spin polarized quasiparticle states exist in the gapped region. Valence band broadening and enhanced localization effects at low temperature indicate strong hybridization of the valence orbitals of Ce atoms with the near neighbor Ge atoms. We find that the intersite interaction between the Ce atoms at high temperature stabilizes the onsite interaction at low temperature that leads to the spin density wave type antiferromagnetism in CeAg2Ge2.

Resonant inelastic x-ray scattering (RIXS) spectra for ladder cuprates

The ladder compound Sr14Cu24O41 is of interest both as a quasi-one-dimensional analog of the superconducting cuprates and as a superconductor in its own right when Sr is substituted by Ca. In order to model resonant inelastic x-ray scattering (RIXS) spectra for this compound, we investigate the simpler SrCu2O3 system in which the crystal structure contains very similar ladder planes. We approximate the LDA dispersion of SrCu2O3 by a Cu only two-band tight-binding model. Strong correlation effects are incorporated by assuming an anti-ferromagnetic ground state. The available angle-resolved photoemission (ARPES) and RIXS data on the ladder compound are found to be in reasonable accord with our theoretical predictions.

Sb2Se3(100) : A strongly anisotropic surface

Interest in antimony selenide (Sb2Se3) has been constantly growing in the recent past, especially for its promising properties for applications in the field of solar energy technologies. Surprisingly, the surface properties of this material, which is built from van der Waals stacked one-dimensional (1D) ribbons, have not been studied in detail yet. Here we demonstrate that Sb2Se3 crystals cleave along the (100) planes. The resulting surface shows a pronounced 1D structure, reflecting the stacking of ribbons in the bulk crystal. The cleaving process leads to the formation of slightly tilted surface domains, with the tilt angles oriented invariably along the ribbon directions, suggesting a strong anisotropy of the internal friction forces. Our angle-resolved photoemission data reveal that the 1D character of the crystalline structure of this material is also reflected in its electronic band structure.

Electronic properties of GaAsBi(001) alloys at low Bi content

Despite its potential in the fields of optoelectronics and topological insulators, experimental electronic band structure studies of Bi-doped GaAs are scarce. The reason is the complexity of growth which tends to leave bulk and in particular surface properties in an undefined state. Here we present an in depth investigation of structural and electronic properties of GaAsBi epilayers grown by molecular beam epitaxy with high (001) crystalline order and well-defined surface structures evident from low-energy electron diffraction. X-ray and ultraviolet photoemission spectrocopy as well as angle-resolved photoemission data at variable photon energies allows to disentangle a Bi-rich surface layer with $(1\times3)$ symmetry from the effects of Bi atoms incorporated in the GaAs bulk matrix. The influence of Bi concentrations up to $\approx 1$\% integrated in the GaAs bulk are visible in angle-resolved photoemission spectra after mild ion bombardment and subsequent annealing steps. Interpretation of our results is obtained via density functional theory simulations of bulk and $\beta 2(2\times 4)$ reconstructed slab geometries with and without Bi. Bi-induced energy shifts in the dispersion of GaAs heavy and light hole bulk bands are evident both in experiment and theory, which are relevant for modulations in the optical band gap and thus optoelectronic applications.

Magnetically driven band shift and metal-insulator transition in spin-orbit-coupled Sr3(Ir1−xRux)2O7

We report a combined infrared and angle-resolved photoemission study of the electronic response of $\mathrm{S}{\mathrm{r}}_{3}{(\mathrm{I}{\mathrm{r}}_{1\ensuremath{-}x}\mathrm{R}{\mathrm{u}}_{x})}_{2}{\mathrm{O}}_{7}$ ($x=0$, 0.22, 0.34). The low-temperature optical conductivities of the three compounds exhibit the characteristic feature of the effective total angular momentum ${J}_{\mathrm{eff}}=1/2$ antiferromagnetic Mott state. As the temperature increases across the antiferromagnetic ordering temperature ${T}_{\mathrm{N}}$, the indirect gap gradually closes whereas the direct gap remains open. In the optical conductivity of $\mathrm{S}{\mathrm{r}}_{3}{(\mathrm{I}{\mathrm{r}}_{0.66}\mathrm{R}{\mathrm{u}}_{0.34})}_{2}{\mathrm{O}}_{7}$ which shows a thermally driven insulator-metal transition at ${T}_{\mathrm{N}}$, a Drude-like response from itinerant carriers is registered in the paramagnetic phase. We observe in angle-resolved photoemission data of $\mathrm{S}{\mathrm{r}}_{3}{(\mathrm{I}{\mathrm{r}}_{0.66}\mathrm{R}{\mathrm{u}}_{0.34})}_{2}{\mathrm{O}}_{7}$ that the valence band shifts continuously toward the Fermi energy with the weakening of the antiferromagnetic order and crosses the Fermi level in the paramagnetic phase. Our findings demonstrate that the temperature-induced metal-insulator transition of the $\mathrm{S}{\mathrm{r}}_{3}{(\mathrm{I}{\mathrm{r}}_{1\ensuremath{-}x}\mathrm{R}{\mathrm{u}}_{x})}_{2}{\mathrm{O}}_{7}$ system should be attributed to a magnetically driven band shift.

Detecting sign-changing superconducting gap in LiFeAs using quasiparticle interference

Using a realistic ten-orbital tight-binding model Hamiltonian fitted to the angle-resolved photoemission (ARPES) data on LiFeAs, we analyze the temperature, frequency, and momentum dependencies of quasiparticle interference (QPI) to identify gap sign changes in a qualitative way, following our original proposal [Phys. Rev. B 92, 184513 (2015)]. We show that all features present for the simple two-band model for the sign-changing $s_{+-}$-wave superconducting gap employed previously are still present in the realistic tight-binding approximation and gap values observed experimentally. We discuss various superconducting gap structures proposed for LiFeAs, and identify various features of these superconducting gaps functions in the quasiparticle interference patterns. On the other hand, we show that it will be difficult to identify the more complicated possible sign structures of the hole pocket gaps in LiFeAs, due to the smallness of the pockets and the near proximity of two of the gap energies.

Topological surface state of α−Sn on InSb(001) as studied by photoemission

We report on the electronic structure of the elemental topological semimetal $\alpha$-Sn on InSb(001). High-resolution angle-resolved photoemission data allow to observe the topological surface state (TSS) that is degenerate with the bulk band structure and show that the former is unaffected by different surface reconstructions. An unintentional $p$-type doping of the as-grown films was compensated by deposition of potassium or tellurium after the growth, thereby shifting the Dirac point of the surface state below the Fermi level. We show that, while having the potential to break time-reversal symmetry, iron impurities with a coverage of up to 0.25 monolayers do not have any further impact on the surface state beyond that of K or Te. Furthermore, we have measured the spin-momentum locking of electrons from the TSS by means of spin-resolved photoemission. Our results show that the spin vector lies fully in-plane, but it also has a finite radial component. Finally, we analyze the decay of photoholes introduced in the photoemission process, and by this gain insight into the many-body interactions in the system. Surprisingly, we extract quasiparticle lifetimes comparable to other topological materials where the TSS is located within a bulk band gap. We argue that the main decay of photoholes is caused by intraband scattering, while scattering into bulk states is suppressed due to different orbital symmetries of bulk and surface states.

Coherent organization of electronic correlations as a mechanism to enhance and stabilize high-TC cuprate superconductivity

Strong diffusive or incoherent electronic correlations are the signature of the strange-metal normal state of the cuprate superconductors, with these correlations considered to be undressed or removed in the superconducting state. A critical question is if these correlations are responsible for the high-temperature superconductivity. Here, utilizing a development in the analysis of angle-resolved photoemission data, we show that the strange-metal correlations don’t simply disappear in the superconducting state, but are instead converted into a strongly renormalized coherent state, with stronger normal state correlations leading to stronger superconducting state renormalization. This conversion begins well above TC at the onset of superconducting fluctuations and it greatly increases the number of states that can pair. Therefore, there is positive feedback––the superconductive pairing creates the conversion that in turn strengthens the pairing. Although such positive feedback should enhance a conventional pairing mechanism, it could potentially also sustain an electronic pairing mechanism.

Constraints on the total coupling strengthto bosons in the iron based superconductors

At present, there is still no consistent interpretation of the normal and superconducting properties of Fe-based superconductors (FeSCs). The strength of the el-el interaction and the role of correlation effects are under debate. Here, we examine several common materials and illustrate various problems and concepts that are generic for all FeSCs. Based on empirical observations and qualitative insight from density functional theory, we show that the superconducting and low-energy thermodynamic properties of the FeSCs can be described semi-quantitively within multiband Eliashberg theory. We account for an important high-energy mass renormalization phenomenologically,and in agreement with constraints provided by thermodynamic, optical, and angle-resolved photoemission data. When seen in this way, all FeSCs with $T_\mathrm{c} <$ 40~K studied so far are found to belong to an {\it intermediate} coupling regime. This finding is in contrast to the strong coupling scenarios proposed in the early period of the FeSC history.We also discuss several related issues, including the role of band shifts as measured by the positions of van Hove singularities, and the nature of a recently suggested quantum critical point in the strongly hole-doped systems AFe$_2$As$_2$ (A = K, Rb, Cs). Using high-precision full relativistic GGA-band structure calculations, we arrive at a somewhat milder mass renormalization in comparison with previous studies. From the calculated mass anisotropies of all Fermi surface sheets, only the $\varepsilon$-pocket near the corner of the BZ is compatible with the experimentally observed anisotropy of the upper critical field. pointing to its dominant role in the superconductivity of these three compounds.

Consistent two-lifetime model for spectral functions of superconductors

Recently it has been found that models with at least two lifetimes have to be considered when analyzing the angle resolved photoemission data in the nodal region of the cuprates [T. Kondo et al., Nat. Commun. 6, 7699 (2015)]. In this paper we compare two such models. First we show that the phenomenological model used by Kondo et al. violates the sum rule for the occupation number. Next we consider the recently proposed model of the so-called Dynes superconductors, wherein the two lifetimes measure the strengths of pair-conserving and pair-breaking processes. We demonstrate that the model of the Dynes superconductors is fully consistent with known exact results and we study in detail the resulting spectral functions. Finally, we show that the spectral functions in the nodal region of the cuprates can be fitted well by the model of the Dynes superconductors.

Persistence of a surface state arc in the topologically trivial phase of MoTe2

The prediction of Weyl fermions in the low-temperature noncentrosymmetric $1{T}^{\ensuremath{'}}$ phase of ${\mathrm{MoTe}}_{2}$ still awaits clear experimental confirmation. Here, we report angle-resolved photoemission (ARPES) data and ab initio calculations that reveal a surface state arc dispersing between the valence and the conduction band, as expected for a Weyl semimetal. However, we find that the arc survives in the high-temperature centrosymmetric $1{T}^{\ensuremath{'}\ensuremath{'}}$ phase. Therefore, a surface Fermi arc is not an unambiguous fingerprint of a topologically nontrivial phase. We have also investigated the surface state spin texture of the $1{T}^{\ensuremath{'}}$ phase by spin-resolved ARPES, and identified additional topologically trivial spin-split states within the projected band gap at higher binding energies.