Photoemission electron microscopy (PEEM) has evolved into an indispensable tool for structural and magnetic characterization of surfaces at the nanometer scale. In strong contrast to synchrotron-radiation-based X-ray PEEM as a leading method for element-specific magnetic properties via magnetic circular dichroism (MCD), laboratory ultraviolet (UV) PEEM has seen limited application with much smaller dichroism effects for in-plane magnetization. Here we introduce darkfield PEEM as a novel approach to enhance MCD contrast in threshold photoemission, enabling efficient MCD imaging with significantly enhanced contrast by an order-of-magnitude for Fe(001). This advancement paves the way for MCD imaging on femtosecond timescales using modern lasers. The experimental results will be quantitatively benchmarked against advanced relativistic photoemission calculations.
The helical Dirac fermions at the surface of topological insulators show a strong circular dichroism which has been explained as being due to either the initial-state spin angular momentum, the initial-state orbital angular momentum, or the handedness of the experimental setup. All of these interpretations conflict with our data from Bi2Te3 which depend on the photon energy and show several sign changes. Our one-step photoemission calculations coupled to ab initio theory confirm the sign change and assign the dichroism to a final-state effect. The spin polarization of the photoelectrons, inste…
Angle-resolved photoemission spectroscopy (ARPES) is the most powerful technique to investigate the electronic band structure of crystalline solids. To completely characterize the electronic structure of topological materials, one needs to go beyond band structure mapping and access information about the momentum-resolved Bloch wavefunction, namely orbitals, Berry curvature, and topological invariants. However, because phase information is lost in the process of measuring photoemission intensities, retrieving the complex-valued Bloch wavefunction from photoemission data has yet remained elusiv…
Although the Ni_4 cluster includes more information regarding the Ni band structure with respect to the Anderson impurity model, it also favors very peculiar ground states which are incompatible with a coherent picture of all dichroism experiments.
The momentum-dependent orbital character in crystalline solids, referred to as orbital texture, is of capital importance in the emergence of symmetry-broken collective phases such as charge density waves as well as superconducting and topological states of matter. By performing extreme ultraviolet multidimensional angle-resolved photoemission spectroscopy for two different crystal orientations linked to each other by mirror symmetry, we isolate and identify the role of orbital texture in photoemission from the transition metal dichalcogenide 1T-TiTe$_2$. By comparing our experimental results w…
We revisit the formulations and simulations of angular distributions in polarization-dependent core-level photoemission spectra of strongly correlated electron systems, in order to explain the recently discovered linear dichroism (LD) in the core-level photoemission of 4f-based rare-earth compounds. Owing to the selection rules for the optical process of core-level excitations, the LD originating from the anisotropic outer localized charge distributions determined by the ground-state orbital symmetry can be observed. Our simulations show that core d-level excitations are essential for the LD i…
We have investigated the effect of imperfect circular polarization on the angle-resolved photoemission spectroscopy signal, using graphene as a prototypical system that can be understood within tight-binding formalism. We found that perfect left- and right-circularly polarized lights give the same photoelectron intensity distribution around a constant energy contour of the graphene $π$ band. On the other hand, upon breaking the purity of the polarization, photoelectron intensity starts to show circular dichroism, which is enhanced with further increasing the imperfection. Our results predict t…
Observing signatures of light-induced Floquet topological states in materials has been shown to be very challenging. Angle-resolved photoemission spectroscopy (ARPES) is well suited for the investigation of Floquet physics, as it allows to directly probe the dressed electronic states of driven solids. Depending on the system, scattering and decoherence can play an important role, hampering the emergence of Floquet states. Another challenge is to disentangle Floquet side bands from laser-assisted photoemission (LAPE), since both lead to similar signatures in ARPES spectra. Here, we investigate …
We have performed x-ray magnetic circular dichroism (XMCD) and valence-band photoemission studies of the diluted ferromagnetic semiconductor Zn$_{1-x}$Cr$_x$Te. XMCD signals due to ferromagnetism were observed at the Cr 2p absorption edge. Comparison with atomic multiplet calculations suggests that the magnetically active component of the Cr ion was divalent under the tetrahedral crystal field with tetragonal distortion along the crystalline a-, b-, and c-axes. In the valence-band spectra, spectral weight near the Fermi level was strongly suppressed, suggesting the importance of Jahn-Teller ef…
We show that the strongly correlated 4f-orbital symmetry of the ground state is revealed by linear dichroism in core-level photoemission spectra as we have discovered for YbRh2Si2 and YbCu2Si2. Theoretical analysis tells us that the linear dichroism reflects the anisotropic charge distributions resulting from crystalline electric field. We have successfully determined the ground-state 4f symmetry for both compounds from the polarization-dependent angle-resolved core-level spectra at a low temperature well below the first excitation energy. The excited-state symmetry is also probed by temperatu…
Pumping graphene with circularly polarized light is the archetype of light-tailoring topological bands. Realizing the induced Floquet-Chern insulator state and tracing clear experimental manifestions has been a challenge, and it has become clear that scattering effects play a crucial role. We tackle this gap between theory and experiment by employing microscopic quantum kinetic calculations including realistic electron-electron and electron-phonon scattering. Our theory provides a direct link to the build-up of the Floquet-Chern insulator state in light-driven graphene and its detection in tim…
Using circularly polarised radiation and a combination of bulk-sensitive hard X-ray photoelectron spectroscopy and X-ray-absorption spectroscopy (XAS) we studied the electronic and magnetic structure of epitaxial Mn$_{1.8}$Co$_{1.2}$Ga thin films. Spin resolved Bloch spectral functions, density of states as well as charge and magnetisation densities were investigated by a first-principles analysis of full potential, fully relativistic Korringa--Kohn--Rostoker calculations of the electronic structure. The valence states were experimentally investigated by using linear dichroism in the angular d…
A first principles approach, based on the real space multiple scattering Green's function method, is presented for spin- and angle-resolved resonant photoemission from magnetic surfaces. It is applied to the Fe(010) valence band photoemission excited with circularly polarized X-rays around the Fe L3 absorption edge. When the photon energy is swept through the Fe 2p-3d resonance, the valence band spectra are strongly modified in terms of absolute and relative peak intensities, degree of spin-polarization and light polarization dependence. New peaks in the spin-polarized spectra are identified a…
Inversion-symmetric crystals are optically isotropic and thus naively not expected to show dichroism effects in optical absorption and photoemission processes. Here, we find a strong linear dichroism effect (up to 42.4%) in the conduction band of inversion-symmetric bilayer MoS$_2$, when measuring energy- and momentum-resolved snapshots of excited electrons by time- and angle-resolved photoemission spectroscopy. We model the polarization-dependent photoemission intensity in the transiently-populated conduction band using the semiconductor Bloch equations and show that the observed dichroism em…
We performed angle-resolved photoemission spectroscopy (ARPES) of bulk 2H-WSe$_2$ for different crystal orientations linked to each other by time-reversal symmetry. We introduce a new observable called time-reversal dichroism in photoelectron angular distributions (TRDAD), which quantifies the modulation of the photoemission intensity upon effective time-reversal operation. We demonstrate that the hidden orbital pseudospin texture leaves its imprint onto TRDAD, due to multiple orbitals interference effects in photoemission. Our experimental results are in quantitative agreement with both tight…
Reexamining Circular Dichroism in Photoemission From a Topological Insulator
Tel Aviv University（特拉维夫大学）；École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；University of West Bohemia（西波希米亚大学）；Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory（斯坦福材料能源科学研究所，SLAC国家加速器实验室）；Geballe Laboratory for Advanced Materials, Stanford University（斯坦福大学高威实验室）；Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory（SLAC国家加速器实验室斯坦福同步辐射光源）
Fe-doped III-V ferromagnetic semiconductors (FMSs) such as (In,Fe)As, (Ga,Fe)Sb, (In,Fe)Sb, and (Al,Fe)Sb are promising materials for spintronic device applications because of the availability of both n- and p-type materials and the high Curie temperatures. On the other hand, (Ga,Fe)As, which has the same zinc-blende crystal structure as the Fe-doped III-V FMSs, shows paramagnetism. The origin of the different magnetic properties in the Fe-doped III-V semiconductors remains to be elucidated. To address this issue, we use resonant photoemission spectroscopy (RPES) and x-ray magnetic circular di…
Co islands and films are characterized by x-ray magnetic circular dichroism photoemission electron microscopy (XMCD-PEEM). The spatial resolution capabilties of the technique together with atomic growth control permit obtaining perfectly flat triangular islands with a given thickness (3 ML), very close to an abrupt spin-reorientation transition. The magnetic domain configurations are found to depend on island size: while small islands can be magnetized in a single-domain state, larger islands show more complex patterns. Furthermore, the magnetization pattern of the larger islands presents a co…
GdNi is a ferrimagnetic material with a Curie temperature Tc = 69 K which exhibits a large magnetocaloric effect, making it useful for magnetic refrigerator applications. We investigate the electronic structure of GdNi by carrying out x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) at T = 25 K in the ferrimagnetic phase. We analyze the Gd M$_{4,5}$-edge ($3d$ - $4f$) and Ni L$_{2,3}$-edge ($2p$ - $3d$) spectra using atomic multiplet and cluster model calculations, respectively. The atomic multiplet calculation for Gd M$_{4,5}$-edge XAS indicates that Gd is triv…
We report on the results of x-ray absorption (XAS), x-ray magnetic circular dichroism (XMCD), and photoemission experiments on {\it n}-type Zn$_{1-x}$Co$_x$O ($x=0.05$) thin film, which shows ferromagnetism at room temperature. The XMCD spectra show a multiplet structure, characteristic of the Co$^{2+}$ ion tetrahedrally coordinated by oxygen, suggesting that the ferromagnetism comes from Co ions substituting the Zn site in ZnO. The magnetic field and temperature dependences of the XMCD spectra imply that the non-ferromagnetic Co ions are strongly coupled antiferromagnetically with each other.
The theoretical description of photoemission spectra of transition metals was greatly improved recently by accounting for the correlations between the d electrons within the local spin density approximation (LSDA) plus dynamical mean field theory (DMFT). We assess the improvement of the LSDA+DMFT over the plain LSDA in x-ray absorption spectroscopy, which --- unlike the photoemission spectroscopy --- is probing unocccupied electronic states. By investigating the L2,3-edge x-ray absorption near-edge structure (XANES) and x-ray magnetic circular dichroism (XMCD) of Fe, Co, and Ni, we find that t…
Absence of magnetic order in epitaxial RuO2 revealed by X-ray linear dichroism
School of Nuclear Science and Technology and National Synchrotron Radiation Laboratory, University of Science and Technology of China（中国科学技术大学核科学与技术学院和国家同步辐射实验室）；Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences（中国科学院上海高等研究院上海同步辐射光源）；Physics department, University of California at Berkeley（加州大学伯克利分校物理系）；State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences（中国科学院大连化学物理研究所分子反应动力学国家重点实验室）；Advanced Light Source, Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室先进光源）；Institute of Physical Science and Information Technology, Anhui University（安徽大学物理科学与信息工程学院）；Nanoelectronics Science and Technology Center, Hefei Innovation Research Institute, Beihang University（北京航空航天大学合肥创新研究院纳米电子科学与技术中心）
This work reports the measurement of magnetic dichroism in angular-resolved photoemission from in-plane magnetized buried thin films. The high bulk sensitivity of hard X-ray photoelectron spectroscopy (HAXPES) in combination with circularly polarized radiation enables the investigation of the magnetic properties of buried layers. HAXPES experiments with an excitation energy of 8 keV were performed on exchange-biased magnetic layers covered by thin oxide films. Two types of structures were investigated with the IrMn exchange-biasing layer either above or below the ferromagnetic layer: one with …
The ferromagnetic to nonferromagnetic (α-β) phase transition in epitaxial MnAs layers on GaAs(100) is studied by x-ray magnetic circular dichroism and x-ray magnetic linear dichroism photoemission electron microscopy in order to elucidate the nature of the controversial nonferromagnetic state of β-MnAs. In the coexistence region of the two phases the β phase shows a clear XMLD signal characteristic of antiferromagnetism. The nature and the possible causes of the elusiveness of this magnetic state are discussed.
We have investigated the electronic structure of ZnO:Mn and ZnO:Mn,N thin films using x-ray magnetic circular dichroism (XMCD) and resonance-photoemission spectroscopy. From the Mn 2$p$$\rightarrow3d$ XMCD results, it is shown that, while XMCD signals only due to paramagnetic Mn$^{2+}$ ions were observed in ZnO:Mn, nonmagnetic, paramagnetic and ferromagnetic Mn$^{2+}$ ions coexist in ZnO:Mn,N. XMCD signals of ZnO:Mn,N revealed that the localized Mn$^{2+}$ ground state and Mn$^{2+}$ state hybridized with ligand hole coexisted, implying $p$-$d$ exchange coupling. In the valence-band spectra, spe…
The origin of the interfacial perpendicular magnetic anisotropy (PMA) induced in the ultrathin Fe layer on the Au(111) surface was examined using synchrotron-radiation-based Mössbauer spectroscopy (MS), X-ray magnetic circular dichroism (XMCD), and angle-resolved photoemission spectroscopy (ARPES). To probe the detailed interfacial electronic structure of orbital hybridization between the Fe 3$d$ and Au 6$p$ bands, we detected the interfacial proximity effect, which modulates the valence-band electronic structure of Fe, resulting in PMA. MS and XMCD measurements were used to detect the interfa…
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 …
A detailed correlative structural, magnetic and chemical analysis of non-stoichiometric cobalt ferrite micrometric crystals was performed by x-ray magnetic circular dichroism combined with photoemission microscopy, low energy electron microscopy, and atomic force microscopy. The vector magnetization at the nanoscale is obtained from magnetic images at different x-ray incidence angles and compared with micromagnetic simulations, revealing the presence of defects which pin the magnetic domain walls. A comparison of different types of defects and the domain walls location suggests that the main s…
Using focused electron-beam-induced deposition (FEBID), we fabricate vertical, platinum-coated cobalt nanowires with a controlled three-dimensional structure. The latter is engineered to feature bends along the height: these are used as pinning sites for domain walls, the presence of which we investigate using X-ray Magnetic Circular Dichroism (XMCD) coupled to PhotoEmission Electron Microscopy (PEEM). The vertical geometry of our sample combined with the low incidence of the X-ray beam produce an extended wire shadow which we use to recover the wire's magnetic configuration. In this transmiss…
We have investigated three-dimensional magnetization structures in numerous mesoscopic Fe/Mo(110) islands by means of x-ray magnetic circular dichroism combined with photoemission electron microscopy (XMCD-PEEM). The particles are epitaxial islands with an elongated hexagonal shape with length of up to 2.5 micrometer and thickness of up to 250 nm. The XMCD-PEEM studies reveal asymmetric magnetization distributions at the surface of these particles. Micromagnetic simulations are in excellent agreement with the observed magnetic structures and provide information on the internal structure of the…
In the field of antiferromagnetic (AFM) spintronics, information about the Néel vector, AFM domain sizes, and spin-flop fields is a prerequisite for device applications but is not available easily. We have investigated AFM domains and spin-flop induced changes of domain patterns in Mn2Au(001) epitaxial thin films by X-ray magnetic linear dichroism photoemission electron microscopy (XMLD-PEEM) using magnetic fields up to 70 T. As-prepared Mn$_2$Au films exhibit AFM domains with an average size $\sim$ 1 $μ$m. Application of a 30T field, exceeding the spin-flop field, along a magnetocrystalline e…
The antiferromagnetic to ferromagnetic phase transition in B2-ordered FeRh is imaged in laterally confined nanopatterned islands using photoemission electron microscopy with x-ray magnetic circular dichroism contrast. The resulting magnetic images directly detail the progression in the shape and size of the FM phase domains during heating and cooling through the transition. In 5 um square islands this domain development during heating is shown to proceed in three distinct modes: nucleation, growth, and merging, each with subsequently greater energy costs. In 0.5 um islands, which are smaller t…
The future developments of three-dimensional magnetic nanotechnology require the control of domain wall dynamics by means of current pulses. While this has been extensively studied in planar magnetic strips (planar nanowires), few reports exist in cylindrical geometry, where Bloch point domain walls are expected to have intriguing properties. Here we report this investigation in cylindrical magnetic Ni nanowires with geometrical notches. Experimental work based on synchrotron X-ray magnetic circular dichroism (XMCD) combined with photoemission electron microscopy (PEEM) indicates that large cu…
