Spin-resolved ARPES Research Articles

Data Acquisition System Based on the Bluesky Suite in the Shanghai Synchrotron Radiation Facility

The Shanghai Synchrotron Radiation Facility Phase-II Project is now under construction and it consists of 16 newly built advanced beamlines. The experiments carried out at these new beamlines tend to be characterized by high flux, multi-mode, ultra-fast frequency, in situ and dynamic loading. To meet these emerging experimental demands of SSRF Phase-II beamlines, the authors have developed a unified and extensible data acquisition system based on Bluesky suite. It has been applied at the BL07U Spatial-resolved and Spin-resolved ARPES and magnetism beamline. The experiment results show that with up to 5 channel signals, the system is capable of collecting total electron yield signals of experimental sample and standard sample, and incident photon flux signals simultaneously. It improves the user experimental efficiency and quality. In addition, thanks to Bluesky suite, all devices can be abstracted as motors or detectors and then represented by a Python object. Therefore, with the architecture, modules and interface developed for BL07U, the system can be extended to more beamlines efficiently and easily.

Altermagnetic surface states: towards the observation and utilization of altermagnetism in thin films, interfaces and topological materials.

The altermagnetism influences the electronic states allowing the presence of non-relativistic spin-splittings. Since altermagnetic spin-splitting is present along specific k-paths of the 3D Brillouin zone, we expect that the altermagnetic surface stateswill be present on specific surface orientations. We unveil the properties of the altermagnetic surface states considering three representative materials belonging to the orthorhombic, hexagonal and tetragonal space groups. We calculate the 2D projected Brillouin zone from the 3D Brillouin zone. We study the surfaces with their respective 2D Brillouin zones establishing where the spin-splittings with opposite sign merge annihilating the altermagnetic properties and on which surfaces the altermagnetism is preserved. Looking at the three principal surface orientations, we find that for several cases two surfaces are blind to the altermagnetism, while the altermagnetism survives for one surface orientation. Which surface preserves the altermagnetism depends also on themagnetic order. We qualitatively show that an electric field orthogonal to the blind surface can activate the altermagnetism. Our projection method was proven for strong altermagnetism, but it will be equivalently valid for recently discovered weak altermagnetism. Our results predict which surfaces to cleave in order to preserve altermagnetism in surfaces or interfaces and this paves the way to observe non-relativistic altermagnetic spin-splitting in thin films via spin-resolved ARPES and to interface the altermagnetism with other collective modes. We open future perspectives for the study of altermagnetic effects on the trivial and topological surface states.

Direct Observation of the Topological Surface State in the Topological Superconductor 2M-WS2.

The quantum spin Hall (QSH) effect has attracted extensive research interest because of the potential applications in spintronics and quantum computing, which is attributable to two conducting edge channels with opposite spin polarization and the quantized electronic conductance of 2e2/h. Recently, 2M-WS2, a new stable phase of transition metal dichalcogenides with a 2M structure showing a layer configuration identical to that of the monolayer 1T' TMDs, was suggested to be a QSH insulator as well as a superconductor with a critical transition temperature of around 8 K. Here, high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES are applied to investigate the electronic and spin structure of the topological surface states (TSS) in the superconducting 2M-WS2. The TSS exhibit characteristic spin-momentum-locking behavior, suggesting the existence of long-sought nontrivial topological states therein. We expect that 2M-WS2 with coexisting superconductivity and TSS might host the promising Majorana bound states.

Observation of Spin-Dependent Dual Ferromagnetism in Perovskite Ruthenates

We performed insitu angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES (SARPES) experiments to investigate the relationship between electronic band structures and ferromagnetism in SrRuO_{3} (SRO) thin films. Our high quality ARPES and SARPES results show clear spin-lifted band structures. The spin polarization is strongly dependent on momentum around the Fermi level, whereas it becomes less dependent at high-binding energies. This experimental observation matches our dynamical mean-field theory results very well. As temperature increases from low to the Curie temperature, spin-splitting gap decreases and band dispersions become incoherent. Based on the ARPES study and theoretical calculation results, we found that SRO possesses spin-dependent electron correlations in which majority and minority spins are localized and itinerant, respectively. Our finding explains how ferromagnetism and electronic structure are connected, which has been under debate for decades in SRO.

Giant Rashba system on a semiconductor substrate with tunable Fermi level: Bi/GaSb(110)–(2×1)

We fabricated spin-polarized surface electronic states with tunable Fermi level from semiconductor to low-dimensional metal in the Bi/GaSb(110)-(2$\times$1) surface using angle-resolved photoelectron spectroscopy (ARPES) and spin-resolved ARPES. The spin-polarized surface band of Bi/GaSb(110) exhibits quasi-one-dimensional character with the Rashba parameter $\alpha _{\rm R}$ of 4.1 and 2.6 eV\AA \ at the $\bar{\Gamma}$ and $\bar{\rm Y}$ points of the surface Brillouin zone, respectively. The Fermi level of the surface electronic state is tuned in situ by element-selective Ar-ion sputtering on the GaSb substrate. The giant Rashba-type spin splitting with switchable metallic/semiconducting character on semiconductor substrate makes this system a promising candidate for future researches in low-dimensional spintronic phenomena.

Angle-resolved photoemission spectroscopy and its application to topological materials

Angle-resolved photoemission spectroscopy (ARPES), an experimental technique based on the photoelectric effect, is arguably the most powerful method for probing the electronic structure of solids. The past decade has witnessed notable progress in ARPES, including the rapid development of soft-X-ray ARPES, time-resolved ARPES, spin-resolved ARPES and spatially resolved ARPES, as well as considerable improvements in energy and momentum resolution. Consequently , ARPES has emerged as an indispensable experimental probe in the study of topological materials, which have characteristic non-trivial bulk and surface electronic structures that can be directly detected by ARPES. Over the past few years, ARPES has had a crucial role in several landmark discoveries in topological materials, including the identification of topological insulators and topological Dirac and Weyl semimetals. In this Technical Review , we assess the latest developments in different ARPES techniques and illustrate the capabilities of these techniques with applications in the study of topological materials.

Giant Rashba splitting of quasi-one-dimensional surface states on Bi/InAs(110)- (2×1)

Electronic states on the Bi/InAs(110)-(2$\times$1) surface and its spin-polarized structure are revealed by angle-resolved photoelectron spectroscopy (ARPES), spin-resolved ARPES, and density-functional-theory calculation. The surface state showed quasi-one-dimensional (Q1D) dispersion and a nearly metallic character; the top of the hole-like surface band is just below the Fermi level. The size of the Rashba parameter ($\alpha_{\rm R}$) reached quite a large value ($\sim$5.5 eV\AA). The present result would provide a fertile playground for further studies of the exotic electronic phenomena in 1D or Q1D systems with the spin-split electronic states as well as for advanced spintronic devices.

Direct observation of high spin polarization in Co2FeAl thin films

We have studied the Co2FeAl thin films with different thicknesses epitaxially grown on GaAs (001) by molecular beam epitaxy. The magnetic properties and spin polarization of the films were investigated by in-situ magneto-optic Kerr effect (MOKE) measurement and spin-resolved angle-resolved photoemission spectroscopy (spin-ARPES) at 300 K, respectively. High spin polarization of 58% (±7%) was observed for the film with thickness of 21 unit cells (uc), for the first time. However, when the thickness decreases to 2.5 uc, the spin polarization falls to 29% (±2%) only. This change is also accompanied by a magnetic transition at 4 uc characterized by the MOKE intensity. Above it, the film’s magnetization reaches the bulk value of 1000 emu/cm3. Our findings set a lower limit on the thickness of Co2FeAl films, which possesses both high spin polarization and large magnetization.

Very efficient spin polarization analysis (VESPA): new exchange scattering-based setup for spin-resolved ARPES at APE-NFFA beamline at Elettra.

Complete photoemission experiments, enabling measurement of the full quantum set of the photoelectron final state, are in high demand for studying materials and nanostructures whose properties are determined by strong electron and spin correlations. Here the implementation of the new spin polarimeter VESPA (Very Efficient Spin Polarization Analysis) at the APE-NFFA beamline at Elettra is reported, which is based on the exchange coupling between the photoelectron spin and a ferromagnetic surface in a reflectometry setup. The system was designed to be integrated with a dedicated Scienta-Omicron DA30 electron energy analyzer allowing for two simultaneous reflectometry measurements, along perpendicular axes, that, after magnetization switching of the two targets, allow the three-dimensional vectorial reconstruction of the spin polarization to be performed while operating the DA30 in high-resolution mode. VESPA represents the very first installation for spin-resolved ARPES (SPARPES) at the Elettra synchrotron in Trieste, and is being heavily exploited by SPARPES users since autumn 2015.

Spin textures of topological surface states at side surfaces ofBi2Se3from first principles

We investigate the spin and spin-orbital textures and electronic structures of topologically protected surface states at side surfaces of ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$ by using slab models within density-functional theory. This is motivated by recent experiments on nanowires, nanoribbons, and nanoplates of ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$ with side surfaces. In particular, two representative surfaces normal to the (111) surface, such as $(1\overline{1}0)$ and $(11\overline{2})$ surfaces, are examined, in the presence of time-reversal symmetry and inversion symmetry. The $(1\overline{1}0)$ surface lying in the mirror plane has twofold $({\mathrm{C}}_{2})$ rotational symmetry, whereas the $(11\overline{2})$ surface has only mirror symmetry. For the $(1\overline{1}0)$ surface, we find that a Dirac cone with strongly anisotropic Fermi velocity is formed at $\mathrm{\ensuremath{\Gamma}}$ with the Dirac point at the Fermi level, and that the spin texture reveals features of Rashba-type combined with Dresselhaus-type spin-orbit coupling. For the $(11\overline{2})$ surface, a Dirac cone is found at either $\mathrm{\ensuremath{\Gamma}}$ or the $Y$ point (along the mirror symmetry axis) below the Fermi level. In this case, the spin texture of the surface states strikingly differs from that of the (111) and $(1\overline{1}0)$ surfaces: (i) the in-plane spin polarization dominantly aligned perpendicular to the [111] direction or the mirror symmetry axis, (ii) the Dresselhaus-type spin texture, and (iii) significant out-of-plane spin polarization away from the mirror symmetry axis. Our findings distinctively differ from the previous works based on the effective bulk model Hamiltonian. Our calculated spin and spin-orbital textures and band structures can be observed by spin-resolved angle-resolved photoemission spectroscopy.

One-dimensional spin texture of Bi(441): Quantum spin Hall properties without a topological insulator

The high index (441) surface of bismuth has been studied using Scanning Tunnelling Microscopy (STM), Angle Resolved Photoemission Spectroscopy (APRES) and spin-resolved ARPES. The surface is strongly corrugated, exposing a regular array of (110)-like terraces. Two surface localised states are observed, both of which are linearly dispersing in one in-plane direction ($k_x$), and dispersionless in the orthogonal in-plane direction ($k_y$), and both of which have a Dirac-like crossing at $k_x$=0. Spin ARPES reveals a strong in-plane polarisation, consistent with Rashba-like spin-orbit coupling. One state has a strong out-of-plane spin component, which matches with the miscut angle, suggesting its {possible} origin as an edge-state. The electronic structure of Bi(441) has significant similarities with topological insulator surface states and is expected to support one dimensional Quantum Spin Hall-like coupled spin-charge transport properties with inhibited backscattering, without requiring a topological insulator bulk.

Photoelectron spectroscopy in a wide hν region from 6 eV to 8 keV with full momentum and spin resolution

High resolution photoelectron spectroscopy is recognized to be a very powerful approach to study surface and bulk electronic structures of various solids by employing different photon energies (hν). In particular, angle resolved photoelectron spectroscopy (ARPES) has progressed dramatically in the last few decades providing useful information on Fermi surface (FS) topology and band dispersions.The information of the electron spin is often decisive to fully understand the electronic properties of many material classes. However, spin-resolved studies by photoelectron spectroscopy were strongly hindered by the low detection efficiency of spin detectors. In the case of surface electronic structures, possible surface degradation with time is a serious problem to discuss intrinsic electronic effects. Therefore rather fast and high efficiency detection is required in the case of surface sensitive spin-resolved ARPES.Two-dimensional (2D) detection is nowadays widely employed in ARPES. In the use of a conventional hemispherical deflection analyzer (HDA), one direction on the 2D detector corresponds to the binding energy EB and the other direction to the emission angle. The novel concept of momentum microscopy, however, directly provides 2D (kx,ky) maps of the photoemission intensities. The reciprocal space image directly represents the cross section through the valence band structure of the sample at a selected energy. By scanning EB, very high resolution three-dimensional EB(kx,ky) maps of the band-dispersion can be obtained with high efficiency.If combined with a 2D imaging spin filter, based on electron reflection at a Au/Ir(001) surface, spin detection efficiency with orders of magnitude higher than other spin detectors is realized, opening a breakthrough in spin-resolved ARPES (SP-ARPES).

Tunnel magnetoresistance scan of a pristine three-dimensional topological insulator

Though the Fermi surface of surface states of a 3D topological insulator (TI) has zero magnetization, an arbitrary segment of the full Fermi surface has a unique magnetic moment consistent with the type of spin-momentum locking in hand. We propose a three-terminal set up, which directly couples to the magnetization of a chosen segment of a Fermi surface hence leading to a finite tunnel magnetoresistance (TMR) response of the nonmagnetic TI surface states, when coupled to spin polarized STM probe. This multiterminal TMR not only provides a unique signature of spin-momentum locking for a pristine TI but also provides a direct measure of momentum resolved out of plane polarization of hexagonally warped Fermi surfaces relevant for $Bi_2Te_3$, which could be as comprehensive as spin-resolved ARPES. Implication of this unconventional TMR is also discussed in the broader context of 2D spin-orbit (SO) materials.

スピン分解ARPESによるBiエッジ構造の1次元Rashba効果の観測

スピン分解ARPESによるBiエッジ構造の1次元Rashba効果の観測

The Rashba-split surface state of Sb2Te3(0 0 0 1) and its interaction with bulk states

The electronic structure of the Sb2Te3(0001) surface exhibits a spin–orbit split surface state in a local energy gap of the projected bulk valence band continuum. We investigate this surface state by high-resolution angle-resolved photoemission spectroscopy (ARPES), spin-resolved ARPES and relativistic one-step photoemission calculations. At low wave vectors the dispersion and spin splitting are well-captured by the predictions of the Rashba model for a two-dimensional electron system. With increasing wave vectors, however, the surface state dispersion becomes more complex and the spin splitting size exhibits an unusual non-monotonic evolution. These deviations from the Rashba model arise from the influence of bulk continuum states near the edge of the projected gap. The spin polarization of the surface state remains intact despite the coupling to bulk states.

Rashba effect of bismuth thin film on silicon studied by spin-resolved ARPES

We report high-resolution spin- and angle-resolved photoemission spectroscopy of bismuth thin film on Si(111) to discuss the spin structure of surface states. We found that, unlike conventional picture of the Rashba splitting, the magnitude of the in-plane spin polarization is asymmetric between two hole pockets across the Brillouin-zone center. In addition, these pockets exhibit a giant out-of-plane spin polarization as large as the in-plane counterpart, which changes the sign across the Γ¯ M¯ line. We also revealed that the spin polarization of the Rashba surface states near the Brillouin-zone boundary (the M¯ point) is gradually reduced on decreasing the film thickness. Our result provides a new pathway to generate and control spin-polarized electrons in the Rashba system.

Rashba effect in antimony and bismuth studied by spin-resolved ARPES

We have performed spin- and angle-resolved photoemission spectroscopy of antimony (Sb) and bismuth (Bi) thin films grown on Si(111) to elucidate the nature of the Rashba effect in the spin-split surface bands. In Sb, we revealed spin polarization with the in-plane vortical texture on an elongated hole-like Fermi surface. The spin polarization is strongly momentum-dependent, almost vanishing at the region away from the Brillouin zone center. Such unusual suppression of the spin polarization is not observed in Bi, pointing to a strong influence from the quantized bulk bands on the surface spin polarization in Sb. The present result strongly suggests that bulk-surface interband scattering should be properly taken into account to understand the Rashba surface states in group-V semimetals.

Separating the bulk and surfacen- top-type transition in the topological insulator GeBi4−xSbxTe7

We identify the multi-layered compound GeBi4Te7 to be a topological insulator with a freestanding Dirac point, slightly above the valence band maximum, using angle-resolved photoemission spectroscopy (ARPES) measurements. The spin polarization satisffies the time reversal symmetry of the surface states, visible in spin-resolved ARPES. For increasing Sb content in GeBi(4-x)SbxTe7 we observe a transition from n- to p-type in bulk sensitive Seebeck coefficient measurements at a doping of x = 0.6. In surface sensitive ARPES measurements a rigid band shift is observed with Sb doping, accompanied by a movement of the Dirac point towards the Fermi level. Between x = 0.8 and x = 1 the Fermi level crosses the band gap, changing the surface transport regime. This difference of the n- to p-type transition between the surface region and the bulk is caused by band bending effects which are also responsible for a non-coexistence of insulating phases in the bulk and in the near surface region.

Electronic and spin structures of solids investigated by means of synchrotron radiation photoemission

Recent progress in research on electronic and spin structures of solids and instrumentation on spin-resolved photoemission at Hiroshima Synchrotron Radiation Center are reported. The fine details of electron dynamics of a typical multiband superconductor Sr2RuO4 were uncovered by high-resolution angle-resolved photoemission spectroscopy (ARPES) with tunable polarizations, and the surface of W(110) was found to have a Dirac-corn-like state of d character with nearly massless energy dispersion by high-resolution ARPES and spin-resolved ARPES (SARPES). The SARPES system with very low energy electron diffraction spin detector and modified VG-SCIENTA R4000 electron analyzer brought a breakthrough in spin detection efficiency as well as energy and angular resolution, and enables precise SARPES measurements for materials that require high energy and angular resolution.

A New Spin on ARPES

The electronic spin degree of freedom is of fundamental importance to all matter, with consequences ranging from the structure of the periodic table to the refrigerator magnet. Understanding the behavior and role of electronic spin in magnetic, correlated, and novel quantum materials is a problem of growing prominence in materials science, both in terms of fundamental science and our ever-growing desire for stricter comprehension and control of electronic spin and magnetic phenomena for technology and energy applications. Spin-resolved ARPES, with its unique simultaneous sensitivity to electronic spin, momentum, and energy, is a powerful method for directly probing the spin dependence of materials and electronic structures of current research interest.