Asymmetric electrostatic dodecapole: compact bandpass filter with low aberrations for momentum microscopy.

Imaging energy filters in photoelectron microscopes and momentum microscopes use spherical fields with deflection angles of 90°, 180° and even 2 × 180°. These instruments are optimized for high energy resolution, and exhibit image aberrations when operated in high transmission mode at medium energy resolution. Here, a new approach is presented for bandpass-filtered imaging in real or reciprocal space using an electrostatic dodecapole with an asymmetric electrode array. In addition to energy-dispersive beam deflection, this multipole allows aberration correction up to the third order. Here, its use is described as a bandpass prefilter in a time-of-flight momentum microscope at the hard X-ray beamline P22 of PETRA III. The entire instrument is housed in a straight vacuum tube because the deflection angle is only 4° and the beam displacement in the filter is only ∼8 mm. The multipole is framed by transfer lenses in the entrance and exit branches. Two sets of 16 different-sized entrance and exit apertures on piezomotor-driven mounts allow selection of the desired bandpass. For pass energies between 100 and 1400 eV and slit widths between 0.5 and 4 mm, the transmitted kinetic energy intervals are between 10 eV and a few hundred electronvolts (full width at half-maximum). The filter eliminates all higher or lower energy signals outside the selected bandpass, significantly improving the signal-to-background ratio in the time-of-flight analyzer.

Circular dichroism in hard X-ray photoelectron diffraction observed by time-of-flight momentum microscopy.

X-ray photoelectron diffraction (XPD) is a powerful technique that yields detailed structural information of solids and thin films that complements electronic structure measurements. Among the strongholds of XPD we can identify dopant sites, track structural phase transitions, and perform holographic reconstruction. High-resolution imaging of kll-distributions (momentum microscopy) presents a new approach to core-level photoemission. It yields full-field kx-ky XPD patterns with unprecedented acquisition speed and richness in details. Here, we show that beyond the pure diffraction information, XPD patterns exhibit pronounced circular dichroism in the angular distribution (CDAD) with asymmetries up to 80%, alongside with rapid variations on a small kll-scale (0.1 Å-1). Measurements with circularly-polarized hard X-rays (hν = 6 keV) for a number of core levels, including Si, Ge, Mo and W, prove that core-level CDAD is a general phenomenon that is independent of atomic number. The fine structure in CDAD is more pronounced compared to the corresponding intensity patterns. Additionally, they obey the same symmetry rules as found for atomic and molecular species, and valence bands. The CD is antisymmetric with respect to the mirror planes of the crystal, whose signatures are sharp zero lines. Calculations using both the Bloch-wave approach and one-step photoemission reveal the origin of the fine structure that represents the signature of Kikuchi diffraction. To disentangle the roles of photoexcitation and diffraction, XPD has been implemented into the Munich SPRKKR package to unify the one-step model of photoemission and multiple scattering theory.

Direct observation of antiferromagnetic parity violation in the electronic structure of Mn2Au.

Using momentum microscopy with sub-µm spatial resolution, allowing momentum resolved photoemission on individual antiferromagnetic domains, we observe an asymmetry in the electronic band structure,E(k)≠E(-k), in Mn2Au. This broken band structure parity originates from the combined time and parity symmetry,PT, of the antiferromagnetic order of the Mn moments, in connection with spin-orbit coupling. The spin-orbit interaction couples the broken parity to the Néel order parameter direction. We demonstrate a novel tool to image the Néel vector direction,N, by combining spatially resolved momentum microscopy withab-initiocalculations that correlate the broken parity with the vectorN.

Time-of-flight photoelectron momentum microscopy with 80-500 MHz photon sources: electron-optical pulse picker or bandpass pre-filter.

The small time gaps of synchrotron radiation in conventional multi-bunch mode (100-500 MHz) or laser-based sources with high pulse rate (∼80 MHz) are prohibitive for time-of-flight (ToF) based photoelectron spectroscopy. Detectors with time resolution in the 100 ps range yield only 20-100 resolved time slices within the small time gap. Here we present two techniques of implementing efficient ToF recording at sources with high repetition rate. A fast electron-optical beam blanking unit with GHz bandwidth, integrated in a photoelectron momentum microscope, allows electron-optical `pulse-picking' with any desired repetition period. Aberration-free momentum distributions have been recorded at reduced pulse periods of 5 MHz (at MAX II) and 1.25 MHz (at BESSY II). The approach is compared with two alternative solutions: a bandpass pre-filter (here a hemispherical analyzer) or a parasitic four-bunch island-orbit pulse train, coexisting with the multi-bunch pattern on the main orbit. Chopping in the time domain or bandpass pre-selection in the energy domain can both enable efficient ToF spectroscopy and photoelectron momentum microscopy at 100-500 MHz synchrotrons, highly repetitive lasers or cavity-enhanced high-harmonic sources. The high photon flux of a UV-laser (80 MHz, <1 meV bandwidth) facilitates momentum microscopy with an energy resolution of 4.2 meV and an analyzed region-of-interest (ROI) down to <800 nm. In this novel approach to `sub-µm-ARPES' the ROI is defined by a small field aperture in an intermediate Gaussian image, regardless of the size of the photon spot.

Readout of an antiferromagnetic spintronics system by strong exchange coupling of Mn2Au and Permalloy.

In antiferromagnetic spintronics, the read-out of the staggered magnetization or Néel vector is the key obstacle to harnessing the ultra-fast dynamics and stability of antiferromagnets for novel devices. Here, we demonstrate strong exchange coupling of Mn2Au, a unique metallic antiferromagnet that exhibits Néel spin-orbit torques, with thin ferromagnetic Permalloy layers. This allows us to benefit from the well-established read-out methods of ferromagnets, while the essential advantages of antiferromagnetic spintronics are only slightly diminished. We show one-to-one imprinting of the antiferromagnetic on the ferromagnetic domain pattern. Conversely, alignment of the Permalloy magnetization reorients the Mn2Au Néel vector, an effect, which can be restricted to large magnetic fields by tuning the ferromagnetic layer thickness. To understand the origin of the strong coupling, we carry out high resolution electron microscopy imaging and we find that our growth yields an interface with a well-defined morphology that leads to the strong exchange coupling.

Suppression of the vacuum space-charge effect in fs-photoemission by a retarding electrostatic front lens.

The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e-e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to -1100 V/mm for Ekin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 µm above the sample surface for Ekin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at Ekin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm2, it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at Ekin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.

Temperature-dependent change of the electronic structure in the Kondo lattice system YbRh2Si2.

The heavy-fermion behavior in intermetallic compounds manifests itself in a quenching of local magnetic moments by developing Kondo spin-singlet many-body states combined with a drastic increase of the effective mass of conduction electrons, which occurs below the lattice Kondo temperatureTK. This behavior is caused by interactions between the strongly localized 4felectrons and itinerant electrons. A controversially discussed question in this context is how the localized electronic states contribute to the Fermi surface upon changing the temperature. One expects that hybridization between the local moments and the itinerant electrons leads to a transition from a small Fermi surface in a non-coherent regime at high temperatures to a large Fermi surface once the coherent Kondo lattice regime is realized belowTK. We demonstrate, using hard x-ray angle-resolved photoemission spectroscopy that the electronic structure of the prototypical heavy fermion compound YbRh2Si2changes with temperature between 100 and 200 K, i.e. far above the Kondo temperature,TK= 25 K, of this system. Our results suggest a transition from a small to a large Fermi surface with decreasing temperature. This result is inconsistent with the prediction of the dynamical mean-field periodic Anderson model and supports the idea of an independent energy scale governing the change of band dispersion.

Single-hemisphere photoelectron momentum microscope with time-of-flight recording.

Photoelectron momentum microscopy is an emerging powerful method for angle-resolved photoelectron spectroscopy (ARPES), especially in combination with imaging spin filters. These instruments record kx-ky images, typically exceeding a full Brillouin zone. As energy filters, double-hemispherical or time-of-flight (ToF) devices are in use. Here, we present a new approach for momentum mapping of the full half-space, based on a large single hemispherical analyzer (path radius of 225 mm). Excitation by an unfocused He lamp yielded an energy resolution of 7.7 meV. The performance is demonstrated by k-imaging of quantum-well states in Au and Xe multilayers. The α2-aberration term (α, entrance angle in the dispersive plane) and the transit-time spread of the electrons in the spherical field are studied in a large pass-energy (6 eV-660 eV) and angular range (α up to ±7°). It is discussed how the method circumvents the preconditions of previous theoretical work on the resolution limitation due to the α2-term and the transit-time spread, being detrimental for time-resolved experiments. Thanks to k-resolved detection, both effects can be corrected numerically. We introduce a dispersive-plus-ToF hybrid mode of operation, with an imaging ToF analyzer behind the exit slit of the hemisphere. This instrument captures 3D data arrays I (EB, kx, ky), yielding a gain up to N2 in recording efficiency (N being the number of resolved time slices). A key application will be ARPES at sources with high pulse rates such as synchrotrons with 500 MHz time structure.

Néel Vector Induced Manipulation of Valence States in the Collinear Antiferromagnet Mn2Au.

The coupling of real and momentum space is utilized to tailor electronic properties of the collinear metallic antiferromagnet Mn2Au by aligning the real space Néel vector indicating the direction of the staggered magnetization. Pulsed magnetic fields of 60 T were used to orient the sublattice magnetizations of capped epitaxial Mn2Au(001) thin films perpendicular to the applied field direction by a spin-flop transition. The electronic structure and its corresponding changes were investigated by angular-resolved photoemission spectroscopy with photon energies in the vacuum-ultraviolet, soft, and hard X-ray range. The results reveal an energetic rearrangement of conduction electrons propagating perpendicular to the Néel vector. They confirm previous predictions on the origin of the Néel spin-orbit torque and anisotropic magnetoresistance in Mn2Au and reflect the combined antiferromagnetic and spin-orbit interaction in this compound leading to inversion symmetry breaking.

Time- and momentum-resolved photoemission studies using time-of-flight momentum microscopy at a free-electron laser.

Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of nonequilibrium electronic processes, transient states in chemical reactions, or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical, and structural analyses requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-electron lasers. We have constructed and optimized a versatile setup commissioned at FLASH/PG2 that combines free-electron laser capabilities together with a multidimensional recording scheme for photoemission studies. We use a full-field imaging momentum microscope with time-of-flight energy recording as the detector for mapping of 3D band structures in (kx, ky, E) parameter space with unprecedented efficiency. Our instrument can image full surface Brillouin zones with up to 7 Å-1 diameter in a binding-energy range of several eV, resolving about 2.5 × 105 data voxels simultaneously. Using the ultrafast excited state dynamics in the van der Waals semiconductor WSe2 measured at photon energies of 36.5 eV and 109.5 eV, we demonstrate an experimental energy resolution of 130 meV, a momentum resolution of 0.06 Å-1, and a system response function of 150 fs.

Retraction: Néel Spin-Orbit Torque Driven Antiferromagnetic Resonance in Mn_{2}Au Probed by Time-Domain THz Spectroscopy [Phys. Rev. Lett. 120, 237201 (2018)].

Retraction of DOI: 10.1103/PhysRevLett.120.237201.

Progress in HAXPES performance combining full-field k-imaging with time-of-flight recording.

An alternative approach to hard-X-ray photoelectron spectroscopy (HAXPES) has been established. The instrumental key feature is an increase of the dimensionality of the recording scheme from 2D to 3D. A high-energy momentum microscope detects electrons with initial kinetic energies up to 8 keV with a k-resolution of 0.025 Å-1, equivalent to an angular resolution of 0.034°. A special objective lens with k-space acceptance up to 25 Å-1 allows for simultaneous full-field imaging of many Brillouin zones. Combined with time-of-flight (ToF) parallel energy recording this yields maximum parallelization. Thanks to the high brilliance (1013 hν s-1 in a spot of <20 µm diameter) of beamline P22 at PETRA III (Hamburg, Germany), the microscope set a benchmark in HAXPES recording speed, i.e. several million counts per second for core-level signals and one million for d-bands of transition metals. The concept of tomographic k-space mapping established using soft X-rays works equally well in the hard X-ray range. Sharp valence band k-patterns of Re, collected at an excitation energy of 6 keV, correspond to direct transitions to the 28th repeated Brillouin zone. Measured total energy resolutions (photon bandwidth plus ToF-resolution) are 62 meV and 180 meV FWHM at 5.977 keV for monochromator crystals Si(333) and Si(311) and 450 meV at 4.0 keV for Si(111). Hard X-ray photoelectron diffraction (hXPD) patterns with rich fine structure are recorded within minutes. The short photoelectron wavelength (10% of the interatomic distance) `amplifies' phase differences, making full-field hXPD a sensitive structural tool.

Néel Spin-Orbit Torque Driven Antiferromagnetic Resonance in Mn_{2}Au Probed by Time-Domain THz Spectroscopy.

We observe the excitation of collective modes in the terahertz (THz) range driven by the recently discovered Néel spin-orbit torques (NSOTs) in the metallic antiferromagnet Mn_{2}Au. Temperature-dependent THz spectroscopy reveals a strong absorption mode centered near 1 THz, which upon heating from 4 to 450 K softens and loses intensity. A comparison with the estimated eigenmode frequencies implies that the observed mode is an in-plane antiferromagnetic resonance (AFMR). The AFMR absorption strength exceeds those found in antiferromagnetic insulators, driven by the magnetic field of the THz radiation, by 3 orders of magnitude. Based on this and the agreement with our theory modeling, we infer that the driving mechanism for the observed mode is the current-induced NSOT. Here the electric field component of the THz pulse drives an ac current in the metal, which subsequently drives the AFMR. This electric manipulation of the Néel order parameter at high frequencies makes Mn_{2}Au a prime candidate for antiferromagnetic ultrafast memory applications.

Writing and reading antiferromagnetic Mn2Au by Néel spin-orbit torques and large anisotropic magnetoresistance.

Using antiferromagnets as active elements in spintronics requires the ability to manipulate and read-out the Néel vector orientation. Here we demonstrate for Mn2Au, a good conductor with a high ordering temperature suitable for applications, reproducible switching using current pulse generated bulk spin-orbit torques and read-out by magnetoresistance measurements. Reversible and consistent changes of the longitudinal resistance and planar Hall voltage of star-patterned epitaxial Mn2Au(001) thin films were generated by pulse current densities of ≃107 A/cm2. The symmetry of the torques agrees with theoretical predictions and a large read-out magnetoresistance effect of more than ≃6% is reproduced by ab initio transport calculations.

Spin-filtered time-of-flight k-space microscopy of Ir - Towards the "complete" photoemission experiment.

The combination of momentum microscopy (high resolution imaging of the Fourier plane) with an imaging spin filter has recently set a benchmark in k-resolution and spin-detection efficiency. Here we show that the degree of parallelization can be further increased by time-of-flight energy recording. On the quest towards maximum information (in earlier work termed "complete" photoemission experiment) we have studied the prototypical high-Z fcc metal iridium. Large partial bandgaps and strong spin-orbit interaction lead to a sequence of spin-polarized surface resonances. Soft X-rays give access to the 4D spectral density function ρ (EB,kx,ky,kz) weighted by the photoemission cross section. The Fermi surface and all other energy isosurfaces, Fermi velocity distribution vF(kF), electron or hole conductivity, effective mass and inner potential can be obtained from the multi-dimensional array ρ by simple algorithms. Polarized light reveals the linear and circular dichroism texture in a simple manner and an imaging spin filter exposes the spin texture. One-step photoemission calculations are in fair agreement with experiment. Comparison of the Bloch spectral function with photoemission calculations uncovers that the observed high spin polarization of photoelectrons from bulk bands originates from the photoemission step and is not present in the initial state.

Hosting of surface states in spin-orbit induced projected bulk band gaps of W(1 1 0) and Ir(1 1 1).

Spin-momentum locking of surface states has attracted great interest in recent years due to envisioned technological applications in the field of spintronics. Normal metal surfaces like W(1 1 0) and Ir(1 1 1) show surface states with energy dispersions and spin-polarization textures, which are reminiscent of topologically non-trivial surface states. In order to understand this phenomenon the connection of bulk and surface states has to be explored. Using time-of-flight momentum microscopy with soft x-ray excitation, we present a comprehensive analysis of the bulk bands of W and Ir. Surface states are determined by the same method with photon excitation in the vacuum ultraviolet region. The superposition of both spectral densities reveals the hosting of surface states within the gap structure of bulk bands projected on the surface Brillouin zone. Quantitative differences in the extension of experimental and theoretical local band gaps indicate an underestimation of electron correlation effects in theory.

Direct 3D mapping of the Fermi surface and Fermi velocity.

We performed a full mapping of the bulk electronic structure including the Fermi surface and Fermi-velocity distribution vF(kF) of tungsten. The 4D spectral function ρ(EB; k) in the entire bulk Brillouin zone and 6 eV binding-energy (EB) interval was acquired in ∼3 h thanks to a new multidimensional photoemission data-recording technique (combining full-field k-microscopy with time-of-flight parallel energy recording) and the high brilliance of the soft X-rays used. A direct comparison of bulk and surface spectral functions (taken at low photon energies) reveals a time-reversal-invariant surface state in a local bandgap in the (110)-projected bulk band structure. The surface state connects hole and electron pockets that would otherwise be separated by an indirect local bandgap. We confirmed its Dirac-like spin texture by spin-filtered momentum imaging. The measured 4D data array enables extraction of the 3D dispersion of all bands, all energy isosurfaces, electron velocities, hole or electron conductivity, effective mass and inner potential by simple algorithms without approximations. The high-Z bcc metals with large spin-orbit-induced bandgaps are discussed as candidates for topologically non-trivial surface states.

Determination of surface and interface magnetic properties for the multiferroic heterostructure Co/BaTiO3 using spleed and arpes.

Co/BaTiO3(0 0 1) is one of the most interesting multiferroic heterostructures as it combines different ferroic phases, setting this way the fundamentals for innovative technical applications. Various theoretical approaches have been applied to investigate the electronic and magnetic properties of Co/BaTiO3(0 0 1). Here we determine the magnetic properties of 3 ML Co/BaTiO3 by calculating spin-polarized electron diffraction as well as angle-resolved photoemission spectra, with both methods being well established as surface sensitive techniques. Furthermore, we discuss the impact of altering the BaTiO3 polarization on the spectra and ascribe the observed changes to characteristic details of the electronic structure.

Microscopic origin of the charge transfer in single crystals based on thiophene derivatives: A combined NEXAFS and density functional theory approach.

We have investigated the charge transfer mechanism in single crystals of DTBDT-TCNQ and DTBDT-F4TCNQ (where DTBDT is dithieno[2,3-d;2',3'-d'] benzo[1,2-b;4,5-b']dithiophene) using a combination of near-edge X-ray absorption spectroscopy (NEXAFS) and density functional theory calculations (DFT) including final state effects beyond the sudden state approximation. In particular, we find that a description that considers the partial screening of the electron-hole Coulomb correlation on a static level as well as the rearrangement of electronic density shows excellent agreement with experiment and allows to uncover the details of the charge transfer mechanism in DTBDT-TCNQ and DTBDT-F4 TCNQ, as well as a reinterpretation of previous NEXAFS data on pure TCNQ. Finally, we further show that almost the same quality of agreement between theoretical results and experiment is obtained by the much faster Z+1/2 approximation, where the core hole effects are simulated by replacing N or F with atomic number Z with the neighboring atom with atomic number Z+1/2.

Spin texture of time-reversal symmetry invariant surface states on W(110).

We find in the case of W(110) previously overlooked anomalous surface states having their spin locked at right angle to their momentum using spin-resolved momentum microscopy. In addition to the well known Dirac-like surface state with Rashba spin texture near the -point, we observe a tilted Dirac cone with circularly shaped cross section and a Dirac crossing at 0.28 × within the projected bulk band gap of tungsten. This state has eye-catching similarities to the spin-locked surface state of a topological insulator. The experiments are fortified by a one-step photoemission calculation in its density-matrix formulation.