Dichroism In Photoemission Research Articles

Electron screening length identifying circular dichroism of photoemission

Circular dichroism angle-resolved photoemission spectroscopy (CD-ARPES) receives much attention due to a resolving power of topological and quantum geometrical nature of two-dimensional systems. We propose the Lippmann-Schwinger photoelectron final state, a scattering solution of the lattice model comprising screened short-range potentials at periodically arranged atomic sites, which characterizes the time-reversed low energy electron diffraction (LEED) state well enough to describe the final state effect entailed in CD-ARPES. We find that, through the final state effect, the electron screening length identifies CD-ARPES not only in the qualitative dichroic polarity but also in the quantitative dichroic strength in various graphene systems like the monolayer graphene, the AA-stacking bilayer graphene, and the twisted bilayer graphene especially in a unified fashion. This finding reveals an interplay between electron screening and circular dichroism and enables to extend the spectroscopic expertise of CD-ARPES to a direct probe of the electron screening.

Photoelectron diffraction for probing valency and magnetism of 4f -based materials: A view on valence-fluctuating EuIr2Si2

We present and discuss the methodology for modeling $4f$ photoemission spectra, $4f$ photoelectron diffraction (PED) patterns, and magnetic dichroism effects for rare-earth-based materials. Using PED and magnetic dichroism in photoemission, we explore the electronic and magnetic properties of the near-surface region of the valence-fluctuating material ${\mathrm{EuIr}}_{2}{\mathrm{Si}}_{2}$. For the Eu-terminated surface, we found that the topmost Eu layer is divalent and exhibits a ferromagnetic order below 10 K. The valency of the next Eu layer, that is the fifth atomic layer, is about 2.8 at low temperature that is close to the valency in the bulk. The properties of the Si-terminated surface are drastically different. The first subsurface Eu layer (fourth atomic layer below the surface) behaves divalently and orders ferromagnetically below 48 K. Experimental data indicate, however, that there is an admixture of trivalent Eu in this layer, resulting in its valency of about 2.1. The next deeper lying Eu layer (eighth atomic layer below the surface) behaves mixed valently, but the estimated valency of 2.4 is notably lower than the value in the bulk. The presented approach and obtained results create a background for further studies of exotic surface properties of $4f$-based materials, and allow us to derive information related to valency and magnetism of individual rare-earth layers in a rather extended area near the surface.

Ultrathin epitaxial cobalt films formed under graphene

The intercalation of cobalt under a graphene monolayer grown on a Ni(111) single crystal film is studied. The experiments are conducted in ultrahigh vacuum. Samples are characterized in situ by low energy electron diffraction, high-energy-resolution photoelectron spectroscopy using synchrotron radiation, and magnetic linear dichroism in photoemission of Co 3p electrons. New data are obtained on the evolution of the atomic and electronic structure and magnetic properties of the system with increasing thickness of the intercalated cobalt layer in the range up to 2 nm. It is shown that a pseudomorphic epitaxial film of Co(111) having magnetization perpendicular to the surface is formed under the grapheme layer during intercalation in an anomalously wide range of thicknesses.

Topological Nonsymmorphic Metals from Band Inversion

We introduce the notion of a band-inverted, topological semimetal in two-dimensional nonsymmorphic crystals. This notion is materialized in the monolayers of MTe$_2$ (M $=$ W, Mo) if spin-orbit coupling is neglected. We characterize the Dirac band touching topologically by the Wilson loop of the non-Abelian Berry gauge field. An additional feature of the Dirac cone in monolayer MTe$_2$ is that it tilts over in a Lifshitz transition to produce electron and hole pockets, a type-II Dirac cone. These pockets, together with the pseudospin structure of the Dirac electrons, suggest a unified, topological explanation for the recently-reported, non-saturating magnetoresistance in WTe$_2$, as well as its circular dichroism in photoemission. We complement our analysis and first-principle bandstructure calculations with an $\textit{ab-initio}$-derived-derived tight-binding model for the WTe$_2$ monolayer.

Angle-resolved photoemission with circularly polarized light in the nodal mirror plane of underdoped Bi2Sr2CaCu2O8+δ superconductor

Unraveling the nature of pseudogap phase in high-temperature superconductors holds the key to understanding their superconducting mechanisms and potentially broadening their applications via enhancement of their superconducting transition temperatures. Angle-resolved photoemission spectroscopy (ARPES) experiments using circularly polarized light have been proposed to detect possible symmetry breaking state in the pseudogap phase of cuprates. The presence (absence) of an electronic order which breaks mirror symmetry of the crystal would in principle induce a finite (zero) circular dichroism in photoemission. Different orders breaking reflection symmetries about different mirror planes can also be distinguished by the momentum dependence of the measured circular dichroism. Here, we report ARPES experiment on an underdoped Bi2Sr2CaCu2O8+δ (Bi2212) superconductor in the Γ (0,0)-Y (π,π) nodal mirror plane using circularly polarized light. No circular dichroism is observed on the level of ∼2% at low temperature, which places a clear constraint on the forms of possible symmetry breaking orders in this sample. Meanwhile, we find that the geometric dichroism remains substantial very close to its perfect extinction such that a very small sample angular offset is sufficient to induce a sizeable dichroic signal. It highlights the importance to establish a perfect extinction of geometric dichroism as a prerequisite for the identification of any intrinsic circular dichroism in this material.

Intercalation synthesis of cobalt silicide under a graphene layer

The silicon intercalation under single-layer graphene formed on the surface of an epitaxial Co(0001) film was investigated. The experiments were performed under conditions of ultra-high vacuum. The thickness of silicon films was varied within the range of up to 1 nm, and the temperature of their annealing was 500°C. The characterization of the samples was carried out in situ by the methods of low-energy electron diffraction, high-energy-resolution photoelectron spectroscopy using synchrotron radiation, and magnetic linear dichroism in photoemission of Co 3p electrons. New data were obtained on the evolution of the atomic and electronic structure, as well as on the magnetic properties of the system with an increase in the amount of intercalated silicon. It was shown that the intercalation under a graphene layer is accompanied by the synthesis of surface silicide Co2Si and a solid solution of silicon in cobalt.

Intercalation synthesis of graphene-capped iron silicide atop Ni(111): Evolution of electronic structure and ferromagnetic ordering

A new method for synthesis of graphene-protected iron silicides has been tested, which consists in formation of graphene on Ni(111) followed by two-step intercalation of the system with Fe and Si. Characterization of the samples was performed in situ by low-energy electron diffraction, angular-resolved photoelectron spectroscopy, core-level photoelectron spectroscopy with synchrotron radiation and magnetic linear dichroism in photoemission of Fe 3p electrons. It is shown, that at 400°C the intercalation of graphene/Ni(111) with iron occurs in a range up to 14ML. The graphene layer strongly interacts with the topmost Fe atoms and stabilizes the fcc structure of the film. The in-plane ferromagnetic ordering of the film has a threshold nature and arises after the intercalation of 5ML Fe due to the thickness-driven spin reorientation transition. Subsequent intercalation of graphene/Fe/Ni(111) with Si leads to the formation of the inhomogeneous system consisted of intercalated and nonintercalated areas. The intercalated islands coalesce at 2ML Si when a Fe-Si solid solution covered with the Fe3Si surface silicide is formed. The Fe3Si silicide is ferromagnetic and has an ordered (√3×√3)R30° structure. The graphene layer is weakly electronically coupled to the silicide phase keeping its remarkable properties ready for use.

Formation and investigation of ultrathin layers of Co2FeSi ferromagnetic alloy synthesized on silicon covered with a CaF2 barrier layer

Ultrathin (∼2nm) films of Co2FeSi ferromagnetic alloy were formed on silicon by solid-phase epitaxy and studied in situ. Experiments were carried out in an ultrahigh vacuum (UHV) using substrates of Si(111) single crystals covered with a 5nm thick CaF2 barrier layer. The elemental and phase composition as well as the magnetic properties of the synthesized films were analyzed by photoelectron spectroscopy using synchrotron radiation and by magnetic linear dichroism in photoemission of Fe 3p and Co 3p electrons. The study shows that the synthesis of the Co2FeSi ferromagnetic alloy occurs in the temperature range of 200–400°C. At higher temperatures, the films become island-like and lose their ferromagnetic properties, as the CaF2 barrier layer is unable to prevent a mass transfer between the film and the Si substrate, which violates the stoichiometry of the alloy.

Magnetic linear dichroism of photoemission from ultrathin manganese films on silicon

The magnetic linear dichroism (MLD) effect in photoemission of Mn 3p electrons was used to study magnetic properties of Mn films (to 2.5 nm thick) grown on the Si(111)-(7 × 7) surface at room temperature and manganese silicide films grown by solid-phase epitaxy. The experiments were performed using linearly polarized light with a photon energy of 130 eV, incident at an angle of 30° to the sample surface. Photoelectron spectra were measured in a narrow solid angle focused along the normal to the surface for two opposite sample magnetization directions in the surface plane, perpendicular to the polarization vector of the light wave. It was shown that the MLD effect characteristic of films with high-temperature ferromagnetism appears after depositing ∼2 nm Mn. The formation of manganese silicides upon annealings of the sample with deposited 2.5 nm Mn results in the disappearance of the MLD effect.

Zen and the art of dichroic photoemission

The discovery of magnetic dichroism in photoemission is celebrating its 25th anniversary this year. Here a review of the underlying general theory for the angular and spin dependence of dichroic core-level photoemission is presented using both a single-particle model and a many-body approach. The established methods of angular momentum coupling offer an elegant and powerful way to analyse the magnetic dichroism and spin polarization in photoemission from core and localized valence levels. In the presence of core-valence interactions one can distinguish different fundamental spectra, which via sum rules are related to physical properties described by coupled tensor operators for spin and orbital moments. By separating the angular dependence from the physical information, different geometries can be distinguished to measure the magnetic circular dichroism (MCD), linear dichroism (LD), circular dichroism in the angular dependence (CDAD), and magnetic linear dichroism in the angular dependence (MLDAD). Various ways to probe the core-hole polarization are discussed, such as using the angular dependence, moment analysis of the spectral distribution, and resonant photoemission decay.

Formation and magnetic properties of the silicon-cobalt interface

Formation of the Si/Co interface and its magnetic properties have been studied by high-resolution photoelectron spectroscopy with synchrotron radiation. The experiments have been performed in situ in superhigh vacuum (5 × 10−10 Torr) with coating thicknesses up to 2 nm. It has been found that, in the initial stage of silicon deposition on the surface of polycrystalline cobalt maintained at room temperature, ultrathin layers of the Co3Si, Co2Si, CoSi, and CoSi2 silicides are formed. The three last phases are nonmagnetic, and their formation gives rise to fast decay of magnetic linear dichroism in photoemission of Co 3p electrons. At deposition doses in excess of ∼0.4 nm Si, a film of amorphous silicon grows on the sample surface. It has been established that the Si/Co interphase boundary is stable at temperatures up to ∼250°C and that further heating of the sample brings about escape of amorphous silicon from the sample surface and initiates processes involving silicide formation.

Electronic structure and magnetic properties of epitaxial FeRh(001) ultrathin films on W(100)

Epitaxial FeRh(100) films (CsCl structure, $\sim 10\ ML\ $ thick), prepared {\it in-situ} on a W(100) single crystal substrate, have been investigated via valence band and core level photoemission. The presence of the temperature-induced, first-order, antiferromagnetic to ferromagnetic (AF$\rightarrow$ FM) transition in these films has been verified via linear dichroism in photoemission from the Fe 3$p$ levels. Core level spectra indicate a large moment on the Fe atom, practically unchanged in the FM and AF phases. Judging from the valence band spectra, the metamagnetic transition takes place without substantial modification of the electronic structure. In the FM phase, the spin-resolved spectra compare satisfactorily to the calculated spin-polarized bulk band structure.

Ferromagnetic alignment of iron nanostructures on the silicon surface

The phase composition, electronic structure, and magnetic properties of nanostructures formed upon deposition of iron on the surface of the Si(556) vicinal face coated by a submonolayer silver film with a √3×√3-Ag structure have been studied using high-energy-resolution photoelectron spectroscopy and analysis of magnetic linear dichroism in photoemission of Fe 3p electrons. The effective thickness of the deposited iron layer is varied from 1 to 25 A. It has been shown that a 1- to 2-A Fe coverage leads to the formation of a metastable iron silicide thin layer with a CsCl-type structure on the surface of the sample. A further deposition of Fe (up to ≈7 A) brings about the formation of chains consisting of nonmagnetic islands of the Fe—Si solid solution on this layer, which are oriented along the steps of the substrate. A ferromagnetic alignment of the system along the surface of the sample appears only at coverages of approximately 10 A, when larger (≈100 nm) iron islands start to grow on the solid solution layer.

10.1007/s11451-008-3026-4

The effect of magnetic linear dichroism in photoemission of Fe 3p electrons was used to investigate the magnetic properties of the Si(100)2 × 1 surface on which iron films up to 10 monolayers thick were deposited at room temperature under ultrahigh vacuum. The experiments were performed with linearly polarized light (at a photon energy of 135 eV) incident at an angle of 30° to the surface. The photoelectron spectra were measured in a narrow solid angle oriented along the normal to the sample surface for two opposite magnetization directions which were parallel to the surface plane and perpendicular to the polarization vector of the light wave. An analysis of the data obtained showed that the effect has a threshold character and appears after deposition of eight Fe monolayers, when the ferromagnetic silicide Fe3Si is formed on the surface.

Photoemission of Mn6Cr single-molecule magnets

We present the status of new experimental studies of X-ray absorption spectroscopy, magnetic circular dichroism in photoemission and spin-resolved photoelectron spectroscopy of Mn6Cr single-molecule magnet systems by use of circularly-polarized synchrotron radiation of the electron storage rings in Maxlab Lund, Sweden und BESSY, Berlin, Germany.

Magnetic dichroism in X-ray photoemission

Dependences of the photoemission spectra of magnetic materials on the degree of circular and linear polarization of the exciting radiation, direction of magnetic moments, and escape angle of photoelectrons have been investigated. Using a simple model, analytical formulas have been obtained for the integrated intensity of the photoemission line as functions of the binding energy of inner levels, exchange splitting, and frequency of the X-ray radiation. The magnitude and the angular distribution of the dichroic signals obtained by the inversion of magnetization, by its rotation through 90°, and by the change in the helicity of the exciting radiation have been determined. It is shown that the dichroism of photoemission makes it possible to study not only ferromagnetic materials, but also antiferromagnetic structures.

Rashba effect at the surfaces of rare-earth metals and their monoxides

We present a systematic study of the Rashba-type spin–orbit interaction at the (0001) surfaces of rare-earth metals and their surface monoxides, specifically of Tb metal and the O/Tb, O/Lu and O/Y surfaces. By means of photoemission experiments and ab initio band-structure calculations, we uncover the influence of this interaction on the surface electronic structure. In turn, the dramatic impact of the charge-density distribution of the surface/interface states on the strength of the Rashba-type spin splitting is demonstrated. We discuss the Rashba effect at magnetic and non-magnetic rare-earth surfaces, and compare with cases where it is negligible. The difference between the Rashba effect and magnetic linear dichroism in photoemission is pointed out to help avoid possible confusion in connection with the simultaneous appearance of these two effects at a magnetic surface.

Spatial dependence of the dichroism of photoemission of Fe1/4TiTe2 upon excitation with circularly polarized radiation

This paper reports on the results of the experimental investigation into the angular dependence of the photoemission of the valence band (the angle-resolved photoelectron spectrum) for the Fe1/4TiTe2 single crystal upon excitation with circularly polarized radiation. The angle-resolved photoelectron spectrum is studied in the vicinity of the Γ point of the Brillouin zone in the two directions ΓK and ΓM with the highest symmetry. The measurements are performed in noncoplanar geometry. The circular dichroism in the photoemission angular distribution is observed over the entire ranges of energies and angles. The magnitude of the dichroism depends on the choice of the band, the binding energy, and the polar angle and varies from 0 at the Γ point to 20%.

Magnetic linear dichroism in photoemission from an ultrathin iron silicide film

The effect of magnetic linear dichroism in photoemission of Fe 3p electrons was used to investigate the magnetic properties of the Si(100)2 × 1 surface on which iron films up to 10 monolayers thick were deposited at room temperature under ultrahigh vacuum. The experiments were performed with linearly polarized light (at a photon energy of 135 eV) incident at an angle of 30° to the surface. The photoelectron spectra were measured in a narrow solid angle oriented along the normal to the sample surface for two opposite magnetization directions which were parallel to the surface plane and perpendicular to the polarization vector of the light wave. An analysis of the data obtained showed that the effect has a threshold character and appears after deposition of eight Fe monolayers, when the ferromagnetic silicide Fe3Si is formed on the surface.

Circular dichroism in photoemission as a fingerprint of surface band structure: The case ofZnSe(001)−c(2×2)

Measurements of circular dichroism in the angular dependence (CDAD) of photoemission from core levels and valence bands of the $\mathrm{ZnSe}(001)\text{\ensuremath{-}}c(2\ifmmode\times\else\texttimes\fi{}2)$ surface are presented. Due to the lowering of the surface symmetry compared to the bulk, the CDAD of surface-related spectral components and of bulk components exhibit different polar variations. We propose a way to identify experimentally surface-related bands in the valence-band photoemission spectra based on these symmetry considerations.