Spin-resolved inverse photoemission of ferromagnetic surfaces

Inverse photoemission (IPE) with spin-polarized electrons provides a way to measure separately the exchange-split majority and minority bands in ferromagnets above the Fermi level. Consequently spin-resolved IPE turns out to be an outstanding technique for obtaining information on surface magnetism: the magnetization of the topmost atomic layer may be investigated by measuring the exchange splitting of electronic states that are localized within the surface layer. Theoretical models of ferromagnetism may be tested by observing the temperature behavior of bands which contribute to the ferromagnetism of the material. The magnetic coupling of an adsorbate to the ferromagnetic substrate may be studied by probing adsorbate-induced bands. Results for the Ni(110) surface serve as an illustration to discuss the status of spin-resolved IPE and its application to the field of surface magnetism.     

Electronic structure of half-metallic ferromagnet Co<Subscript>2</Subscript>MnSi at high-pressure

In this study, first principles calculation results of the half-metallic ferromagnetic Heusler compound Co₂MnSi are presented. All calculations are based on the spin-polarized generalized gradient approximation (σ-GGA) of the density functional theory and ultrasoft pseudopotentials with plane wave basis. Electronic structure of related compound in cubic L2₁ structure is investigated up to 95 GPa uniform hydrostatic pressure. The half-metal to metal transition was observed around ~70 GPa together with downward shift of the conduction band minimum (CBM) and a linear increase of direct band gap of minority spins at Γ-point with increasing pressure. The electronic density of states of minority spins at Fermi level, which are mainly due to the cobalt atoms, become remarkable with increasing pressure resulting a sharp decrease in spin polarization ratio. It can be stated that the pressure affects minority spin states rather than that of majority spins and lead to a slight reconstruction of minority spin states which lie below the Fermi level. In particular, energy band gap of minority spin states in equilibrium structure is obviously not destroyed, but the Fermi level is shifted outside the gap.     

Spin-orbit hybridization points in the face-centered-cubic cobalt band structure

Linear magnetic dichroism is observed in spin-, time-, and energy-resolved two-photon photoemission from valence bands of epitaxial fcc cobalt on Cu(001). With image-potential states as spectator states we identify initial bulk and surface states with minority spin character as the source for dichroic intensities and apparent dichroic lifetimes. Excellent agreement with ab initio fully relativistic calculations of the cobalt fcc band structure allows us to precisely determine spin-orbit hybridization points close to the Fermi level. These spin hot spots enhance spin-flip scattering by several orders of magnitude and are therefore assumed to be crucial in ultrafast demagnetization.     

Spin- and angle-resolved photoemission from ferromagnetic Fe(001)

For near-normal photoemission from ferromagnetic Fe(001) excited by linearly polarized synchrotron radiation, energy-resolved spin polarization and intensity distribution have been measured at 60 eV photon energy. Calculations using a one-step theory of photoemission consistently reproduce. the present spin-resolved data as well as earlier spin-averaged measurements. The quasi-particle exchange splitting deduced from the data is 2 eV. The agreement with band structure calculations is suggested to be coincidental due to a compensation of real and imaginary self-energy corrections.     

Three-dimensional spin rotations at the Fermi surface of a strongly spin-orbit coupled surface system

The spin texture of the metallic two-dimensional electron system (sqrt[3]×sqrt[3])-Au/Ge(111) is revealed by fully three-dimensional spin-resolved photoemission, as well as by density functional calculations. The large hexagonal Fermi surface, generated by the Au atoms, shows a significant splitting due to spin-orbit interactions. The planar components of the spin exhibit a helical character, accompanied by a strong out-of-plane spin component with alternating signs along the six Fermi surface sections. Moreover, in-plane spin rotations toward a radial direction are observed close to the hexagon corners. Such a threefold-symmetric spin pattern is not described by the conventional Rashba model. Instead, it reveals an interplay with Dresselhaus-like spin-orbit effects as a result of the crystalline anisotropies.     

单层GaSe表面Fe原子吸附体系电子自旋性质调控

Ⅲ族金属单硫化物因其优越的光电和自旋电子特性而备受关注,实现对其自旋性质的有效调控是发展器件应用的关键.本文采用密度泛函理论系统地研究了GaSe表面Fe原子吸附体系的几何构型及自旋电子特性.Fe/GaSe体系中Fe吸附原子与最近邻Ga,Se原子存在较强的轨道耦合效应,使体系呈现100%自旋极化的半金属性.其自旋极化贡献主要来源于Fe-3d电子的转移及Fe-3d,Se-4p和Ga-4p轨道杂化效应.对于Fe双原子吸附体系,两Fe原子之间的自旋局域导致原本从Fe转移至GaSe的自旋极化电荷量减少,从而费米能级附近的单自旋通道转变为双自旋通道,费米能级处的自旋极化率转变为0.研究结果揭示了Fe_n/GaSe吸附体系自旋极化特性的形成和转变机制,可为未来二维自旋纳米器件的设计与构建提供参考.     

Direct observation of the mass renormalization in SrVO3 by angle resolved photoemission spectroscopy

Band dispersions and Fermi surfaces of the three-dimensional Mott-Hubbard system SrVO3 are directly observed by angle-resolved photoemission spectroscopy. An observed spectral weight distribution near the Fermi level (E(F)) shows cylindrical Fermi surfaces as predicted by band-structure calculations. By comparing the experimental results with calculated surface electronic structures, we conclude that the obtained band dispersion reflects the bulk electronic structure. The enhanced effective electron mass obtained from the energy band near E(F) is consistent with the bulk thermodynamic properties and hence with the normal Fermi-liquid behavior of SrVO3.     

Spin-polarized surface states on Fe-deposited Au(111) surface: A theoretical study

We have studied electronic structure of Fe-deposited Au(111) by performing ab initio density functional theory calculations. We find that the magnetic moment on the deposited Fe layer is enhanced as compared to that in bulk iron. We observe a large number of new states on the Fe-deposited surface — one of which is in the majority spin channel having similar dispersion to that on the clean surface, and others in the minority spin channel. The effective mass of electrons in surface states near the Fermi level increases on Fe deposition. The electronic properties are found to be insensitive to the stacking of near-surface layers. We need to use very thick slabs in our calculations to avoid splitting of surface states due to spurious interactions between the two surfaces of the slab. Using the local density of states profiles for different surface states, we conclude that in scanning tunneling microscope experiments one can detect two of the surface states — one in the majority channel below the Fermi level, and another in the minority channel appearing just above the Fermi energy. We compare our results to those from scanning tunneling spectroscopy experiments.     

Charge-transfer at silver/phthalocyanines interfaces

Valence band photoemission spectroscopy (VB-PES) and inverse photoemission spectroscopy (IPES) were employed to determine the occupied and unoccupied density of states upon silver deposition onto layers of two phthalocyanines (H₂Pc and CuPc). The two different Pc molecules give rise to very distinct behaviour already during the initial stage of silver deposition. While in the CuPc case no shift occurs in the energy levels, the H₂Pc highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) are shifting simultaneously by 0.3 eV, i.e., the HOMO shifts away from the Fermi level while LUMO shifts towards the Fermi level. As the silver quantity increases the HOMO levels of both Pcs are shifting towards the Fermi level. When the Fermi level is resolved in the VB spectra, the characteristic features of H₂Pc and CuPc are smeared out to some extent. Shifts in HOMO and LUMO energy positions as well as changes in line shapes are discussed in terms of charge-transfer and chemical reactions at the interfaces.     

Conduction electron distributions in europium and gadolinium by soft x-ray spectroscopy

A study of the 5d6s conduction band in Eu and Gd by soft X-ray spectroscopy is presented. Our observation that the density of occupied d states is lower for Eu than for Gd is supported by band structure calculations. For Gd, the convolution integrals between the 3p_3/2 inner level Lorentzian distribution and the A.P.W. densities of states are compared with our experimental M_m spectra. The position of the occupied 4f states with respect to the Fermi level is determined, compared with X-ray photoemission data and discussed for both metals.     

Realization of a spin-polarized two-dimensional electron gas via image-potential-induced surface states

Electrons in image-potential-induced surface states form a two-dimensional electron gas in front of the surfaces. In the case of ferromagnets, their binding energies as well as lifetimes depend on the orientation of their spin magnetic moment with respect to the magnetization direction. Various experiments with inverse photoemission and two-photon photoemission to detect the spin dependence of image states are reviewed. A new and successful approach to achieve and detect a spin-polarized two-dimensional electron gas is presented, namely polarization-dependent and spin-resolved two-photon photoemission. Additional time resolution opens the way to study spin-dependent electron dynamics.     

Spin-resolved impurity phase shifts in CuMn

Information deduced from spin-resolved scattering and exchange energy measured via the de Haas - van Alphen effect allows an examination of two recent calculations of the Mn magnetic impurity resonance in Cu. The resulting d-number N_d and spin S are in good agreement, lending further evidence for nearly integer number of d-electrons and a small $\text{long-range}$ magnetic moment. A substantial difference in majority spin density at E_F leads to an explanation for the non-observation of the Mn resonance in optical and photoemission measurements on CuMn.     

Spin-orbit coupling in the Mott insulator Ca(2)RuO(4)

O 1s x-ray absorption study of the Mott insulator Ca(2)RuO(4) shows that the orbital population of the 4d t(2g) band dramatically changes with temperature. In addition, spin-resolved circularly polarized photoemission study of Ca(2)RuO(4) shows that a substantial orbital angular momentum is induced in the Ru 4d t(2g) band. Based on the experimental results and model Hartree-Fock calculations, we argue that the cooperation between the strong spin-orbit coupling in the Ru 4d t(2g) band and the small distortion of the RuO(6) octahedra causes the interesting changeover of the spin and orbital anisotropy as a function of temperature.     

Electronic structure of cubic uranium compounds

Self-consistent cellular multiple scattering techniques and photoemission energy distribution curves obtained at 20<hv<80 eV are used to study the density of states of UN and US. The calculations are based on a model using a finite cluster of atoms in a condensed-matter-like boundary potential. The main results refer to the mixing of thes, p, d, andf-states of uranium into a valence and a conduction band. Thef-states form orbitals with the ligands, within the valence and conduction bands. In the nitride the amount off character in the valence band is only 0.3 electrons and thef electrons are in two resonant levels (of each spin) in the conduction band. Only the first of these levels is occupied for the local, alternate from atom to atom, majority spin. In the sulfide the amount off character in the valence band is 0.59 electrons and the rest of thef-levels are in a resonance state (of majority spin) at the beginning of the conduction band. The conduction band is mainly of localized uranium 6d character. The theoretical results compare favorably with the photoemission data reported here.     

In situ photoemission study of Pr1-xCaxMnO3 epitaxial thin films with suppressed charge fluctuations

We have performed an in situ photoemission study of Pr1-xCaxMnO3 (PCMO) thin films grown on LaAlO3 (001) substrates and observed the effect of epitaxial strain on the electronic structure. We found that the chemical potential shifted monotonically with doping, unlike bulk PCMO, implying the disappearance of incommensurate charge fluctuations of bulk PCMO. In the valence-band spectra, we found a doping-induced energy shift toward the Fermi level (EF) but there was no spectral weight transfer, which was observed in bulk PCMO. The gap at EF was clearly seen in the experimental band dispersions determined by angle-resolved photoemission spectroscopy and could not be explained by the metallic band structure of the C-type antiferromagnetic state, probably due to localization of electrons along the ferromagnetic chain direction or due to another type of spin-orbital ordering.     

Valence surface electronic states on Ge(001)

The optical, electrical, and chemical properties of semiconductor surfaces are largely determined by their electronic states close to the Fermi level (E{F}). We use scanning tunneling microscopy and density functional theory to clarify the fundamental nature of the ground state Ge(001) electronic structure near E{F}, and resolve previously contradictory photoemission and tunneling spectroscopy data. The highest energy occupied surface states were found to be exclusively back bond states, in contrast to the Si(001) surface, where dangling bond states also lie at the top of the valence band.     

Electronic structure reconstruction of CaFe2As2 in the spin density wave state

The electronic structure of CaFe₂As₂, a parent compound of iron-based superconductors, is studied with high-resolution angle-resolved photoemission spectroscopy. The electronic structure of CaFe₂As₂ in the paramagnetic state is consistent with that of density-functional theory calculations. We show that the electronic structure of this compound is significantly reconstructed when entering the spin density wave state. We could resolve two hole-like pockets and four electron-like pockets around the (0, 0) point, and one electron-like pocket surrounded with a pair of electron- and hole-like pockets around the (π, π) point in the spin density wave state. Therefore, the complicated Fermi surface topology and electronic structure near Fermi surface of CaFe₂As₂ illustrate that there exists unconventional electronic reconstruction in the spin density wave state, which cannot be explained by the band folding and Fermi surface nesting pictures.     

UV-photoemission measurements on erbium and samarium

Photoemission measurements have been made on samarium and erbium in the photon energy range 4 to 21 eV. The photoelectron energy distributions are dominated by electron emission from valence band states whereas emission from 4f-states is unimportant. The width and energy of the occupied and unoccupied 5d-bands has been determined as well as the energy relative to the Fermi level of the bottom of the valence band. A model for the unscattered yield is presented allowing a determination of the hot electron scattering length for some rare-earths using available optical and photoemission data.     

Observation of the self-convolved spin-split valence band density of states in MVV Auger decay from Fe(100)

By spin-resolved photoemission with synchrotron radiation we have investigated the Auger electrons from Fe(100) above the 3 p-3d resonance. The observed majority- and minority-spin Auger electrons have the expected kinetic energy independent on photon energy and without noticeable reduction because of correlation effects. The spin-resolved Auger electron energy distributions resemble convolutions of theoretical density of states curves of appropriate spin direction.