Bulk spin polarization of magnetite from spin-resolved hard x-ray photoelectron spectroscopy

Physical review / B 104(4), 045129 (1-10) (2021). doi:10.1103/PhysRevB.104.045129

New HAXPES Applications at PETRA III

The application of photoelectron spectroscopy using hard X-rays (HAXPES) is becoming increasingly popular as a powerful spectroscopic tool in materials science. The success of HAXPES lies in the fa...

Space-, time- and spin-resolved photoemission

Journal of electron spectroscopy and related phenomena 200, 94 - 118 (2015). doi:10.1016/j.elspec.2015.05.016

Near-Edge X-ray Absorption Fine Structure Investigation of the Quasi-One-Dimensional Organic Conductor (TMTSF)2PF6

We present high-resolution near-edge X-ray absorption fine structure (NEXAFS) measurements at the P L2/3-edges, F K-edge, C K-edge and Se M2/3-edges of the quasi-one-dimensional (1D) conductor and superconductor (TMTSF)2PF6. NEXAFS allows probing the donor and acceptor moieties separately; spectra were recorded between room temperature (RT) and 30 K at normal incidence. Spectra taken around RT were also studied as a function of the angle (θ) between the electric field of the X-ray beam and the 1D conducting direction. In contrast with a previous study of the S L2/3-edges spectra in (TMTTF)2AsF6, the Se M2/3-edges of (TMTSF)2PF6 do not exhibit a well resolved spectrum. Surprisingly, the C K-…

Correction of the deterministic part of space–charge interaction in momentum microscopy of charged particles

Abstract Ultrahigh spectral brightness femtosecond XUV and X-ray sources like free electron lasers (FEL) and table-top high harmonics sources (HHG) offer fascinating experimental possibilities for analysis of transient states and ultrafast electron dynamics. For electron spectroscopy experiments using illumination from such sources, the ultrashort high-charge electron bunches experience strong space–charge interactions. The Coulomb interactions between emitted electrons results in large energy shifts and severe broadening of photoemission signals. We propose a method for a substantial reduction of the effect by exploiting the deterministic nature of space–charge interaction. The interaction…

Spinovo rozlisena time-of-flight k-reozlisena fotoemissia Ir-- Kompletny fotoemissny experiment.

Ultramicroscopy 183, 19 - 29 (2017). doi:10.1016/j.ultramic.2017.06.025

Momentum-resolved photoelectron absorption in surface barrier scattering on Ir(111) and graphene/Ir(111)

Physical review / B 96(15), 155108 (2017). doi:10.1103/PhysRevB.96.155108

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

Review of scientific instruments 92(5), 053703 (2021). doi:10.1063/5.0046567

Rashba splitting of the Tamm surface state on Re(0001) observed by spin-resolved photoemission and scanning tunneling spectroscopy

Physical review research 2(1), 013296 (2020). doi:10.1103/PhysRevResearch.2.013296

Energy- and k -resolved mapping of the magnetic circular dichroism in threshold photoemission from Co films on Pt(111)

The magnetic circular dichroism in threshold photoemission (TPMCD) for perpendicularly magnetized fcc Co films on Pt(111) has been revisited. A complete mapping of the spectral function $I({E}_{B},{k}_{x},{k}_{y})$ (binding energy ${E}_{B}$, momentum parallel to surface ${k}_{x}$, ${k}_{y}$) and the corresponding TPMCD asymmetry distribution ${A}_{\mathrm{MCD}}({E}_{B},{k}_{x},{k}_{y})$ has been performed for one-photon and two-photon photoemission using time-of-flight momentum microscopy. The experimental results allow distinguishing direct from indirect transitions. The measurements reveal clear band features of direct transitions from bulk bands that show a nontrivial asymmetry pattern. …

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

AbstractWe 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 "Equation missing"-point, we observe a tilted Dirac cone with circularly shaped cross section and a Dirac crossing at 0.28 × "Equation missing" "Equation missing" 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.

Soft X-ray emission spectroscopy used for the characterization of a-C and CNx thin films

Abstract We present the results of a soft X-ray emission spectroscopy study of a-C and CNx films on a Si(100) substrate. Also for the characterization of the homogeneity in depth of these films electron energy loss spectroscopy measurements with localization better than 4 nm were carried out. In case of CNx films the highest diamond-like modification occurs in the region close to the Si(100) substrate. The film density decreases with increasing distance from the substrate and becomes almost constant in range of thicknesses more than ~ 2 nm.

Electronic structure of large disc-type donors and acceptors

Searching for new pi-conjugated charge-transfer systems, the electronic structure of a new acceptor-donor pair derived from coronene (C(24)H(12)) was investigated by ultraviolet photoelectron spectroscopy (UPS). The acceptor coronene-hexaone (C(24)H(6)O(6), in the following abbreviated as COHON) and the donor hexamethoxycoronene (C(30)H(24)O(6), abbreviated as HMC) were adsorbed as pure and mixed phases on gold substrates. At low coverage, COHON adsorption leads to the appearance of a charge-transfer induced interface state 1.75 eV below the Fermi energy. At multilayer coverage the photoemission intensity of the interface state drops and the valence spectrum of neutral COHON appears. The sa…

Relation between spin–orbit induced spin polarization, Fano-effect and circular dichroism in soft x-ray photoemission

A Feynman diagram analysis of photoemission probabilities suggests a relation between two final-state spin polarization effects, the optical spin-orientation originating from the interaction with circularly polarized light ([Formula: see text], Fano effect) and the spin polarization induced by the spin-orbit scattering ([Formula: see text], Mott effect). The analysis predicts that [Formula: see text] is proportional to the product of [Formula: see text] and the circular dichroism in the angular distribution (CDAD) of photoelectrons. To confirm this prediction, the spin polarization of photoelectrons excited by soft x-ray radiation from initial spin-degenerate bulk states of tungsten using t…

Donor–anion interactions at the charge localization and charge ordering transitions of (TMTTF)2AsF6 probed by NEXAFS

High-resolution near-edge X-ray absorption fine structure (NEXAFS) measurements at the As M-edge, F K-edge and S L-edge of the Fabre salt (TMTTF)2AsF6 were performed from room temperature (RT) to 90 K, allowing to reach the charge localization regime below Tρ ≈ 230 K and to cross the charge ordering (CO) transition at TCO ≈ 102 K. The F K-edge and S L-edge spectra exhibit several transitions which have been indexed on the basis of first-principles DFT calculations. Upon cooling from RT significant energy shifts up to +0.8 eV and -0.4 eV were observed in transitions exhibited by the F 1s and S 2p spectra respectively, while the As 3p doublet does not show a significant shift. Opposite energy…

Crystal growth, structure, magnetic properties and theoretical exchange interaction calculations of Cu2MnBO5

Single crystals of ludwigite Cu2MnBO5 were synthesized by flux growth technique. The detailed structural and magnetic characterizations of the synthesized samples have been carried out. The cations composition of the studied crystal was determined using X-ray diffraction and EXAFS technique, the resulting composition differ from the content of the initial Mn2O3–CuO components of the flux. Magnetic susceptibility measurements and the calculations of the exchange integrals in frameworks of indirect coupling model revealed that monoclinic distortions strongly affect exchange interactions and appearance of magnetic ordering phase at the temperature T=93 K. The hypothesis of the existence of sev…

Charge transfer in the novel donor-acceptor complexes tetra- and hexamethoxypyrene with tetracyanoquinodimethane studied by HAXPES

Abstract The effect of charge transfer (CT) in complexes of the donors tetra - and hexamethoxyprene ( TMP and HMP ) with the classical acceptor tetracyanoquinodimethane ( TCNQ ) was studied using hard X-ray photoemission (HAXPES). Microcrystals of the complex were grown via vapour diffusion from donor–acceptor mixtures. The bulk sensitivity of HAXPES at a photon energy of 6 keV completely eliminates the problem of surface contamination for such delicate organic materials grown from solution. The donor molecules were produced using a novel synthesis route functionalizing polycyclic aromatic hydrocarbons at their periphery. For comparison, spectra were also taken from thin-film samples of the…

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 w…

Orbital-Resolved Partial Charge Transfer from the Methoxy Groups of Substituted Pyrenes in Complexes with Tetracyanoquinodimethane—A NEXAFS Study

It is demonstrated that the near-edge X-ray absorption fine structure (NEXAFS) provides a powerful local probe of functional groups in novel charge transfer (CT) compounds and their electronic properties. Microcrystals of tetra-/hexamethoxypyrene as donors with the strong acceptor tetracyano-p-quinodimethane (TMP/HMP-TCNQ) were grown by vapor diffusion. The oxygen and nitrogen K-edge spectra are spectroscopic fingerprints of the functional groups in the donor and acceptor moieties, respectively. The orbital selectivity of the NEXAFS pre-edge resonances allows us to precisely elucidate the participation of specific orbitals in the charge transfer process. Upon complex formation, the intensit…

Band structure tuning of Heusler compounds: Spin- and momentum-resolved electronic structure analysis of compounds with different band filling

Physical review / B 103(5), 054407 (2021). doi:10.1103/PhysRevB.103.054407

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

Journal of synchrotron radiation 26(6), 1996-2012 (2019). doi:10.1107/S1600577519012773

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 single hemispherical analyzer (path radius 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 alpha-square-aberration term (alpha: entrance an…

Spectral Measurement of Photon Emission from Individual Gold Nanoparticles Using Scanning Tunneling Microscopy

The light emission spectra of individual Au nanoparticles induced by a scanning tunneling microscope (STM) have been investigated. Two-dimensional ensembles of tunnel-coupled Au particles were prepared by thermal evaporation onto a native oxide silicon wafer in ultrahigh vacuum (10 – 9 mbar). Our STM measurements show a single peak at photon energy 1.6 eV in the tunneling mode and two peaks at 2.2 eV (connected with the Mie plasmon) and 1.45 eV (a new peak which was not discussed in literature before) in the field emission mode.

Multi-MHz time-of-flight electronic bandstructure imaging of graphene on Ir(111)

In the quest for detailed spectroscopic insight into the electronic structure at solid surfaces in a large momentum range, we have developed an advanced experimental approach. It combines the 3D detection scheme of a time-of-flight momentum microscope with an optimized filling pattern of the BESSY II storage ring. Here, comprehensive data sets covering the full surface Brillouin zone have been used to study faint substrate-film hybridization effects in the electronic structure of graphene on Ir(111), revealed by a pronounced linear dichroism in angular distribution. The method paves the way to 3D electronic bandmapping with unprecedented data recording efficiency.

Mapováni spinů povrchových a bulkových Rashba stavů v tenkých vrstvách feroelektrického α-GeTe(111)

Rozbíjení inverzní symetrie ve fereeleRashba efekt; Fotoemisse; DFTktrickém polovodiči způsobuje děleni stavů, tzv Rashba efekt. V tomto článku ukazujeme kompletně mapování spinové polarizace těchto Rashba stavů za pomoci spinovo rozlišené fotoemisse. The breaking of bulk inversion symmetry in ferroelectric semiconductors causes a Rashba-type spin splitting of electronic bulk bands. This is shown by a comprehensive mapping of the spin polarization of the electronic bands in ferroelectric α- GeTe(111) films using a time-of-flight momentum microscope equipped with an imaging spin filter that enables a simultaneous measurement of more than 10 000 data points. The experiment reveals an opposite…

Néel Vector Induced Manipulation of Valence States in the Collinear Antiferromagnet Mn 2 Au

The coupling of real and momentum space is utilized to tailor electronic properties of the collinear metallic antiferromagnet Mn2Au by aligning the real space Neel vector indicating the direction o...

Temperature-Dependent Change of the Electronic Structure in the Kondo Lattice System $YbRh_{2}Si_{2}$

Seminar, Deutschland; Journal of physics / Condensed matter 00(00), 1-20 (2021). doi:10.1088/1361-648X/abe479

Site-specific atomic order and band structure tailoring in the diluted magnetic semiconductor (In,Ga,Mn)As

Physical review / B 103(7), 075107 (1-13) (2021). doi:10.1103/PhysRevB.103.075107

Formation of an intermolecular charge-transfer compound in UHV codeposited tetramethoxypyrene and tetracyanoquinodimethane

Ultrahigh vacuum (UHV)-deposited films of the mixed phase of tetramethoxypyrene and tetracyanoquinodimethane $({\text{TMP}}_{1}{\text{-TCNQ}}_{1})$ on gold have been studied using ultraviolet photoelectron spectroscopy (UPS), x-ray diffraction (XRD), infrared (IR) spectroscopy, and scanning tunneling spectroscopy (STS). The formation of an intermolecular charge-transfer (CT) compound is evident from the appearance of new reflexes in XRD (${d}_{1}=0.894\text{ }\text{nm}$ and ${d}_{2}=0.677\text{ }\text{nm}$). A softening of the CN stretching vibration (redshift by $7\text{ }{\text{cm}}^{\ensuremath{-}1}$) of TCNQ is visible in the IR spectra, being indicative of a CT on the order of $0.3e$ f…

Dirakův kužel a pseudogapped hustota stavů v topologické polovině Heuslerovy sloučeniny YPtBi

Topologické izolátory (Tis) jsou zajímavé materiály, které vykazují nebývalé vlastnosti. . Zde jsme prozkoumali sloučeniny YPtBi jako příklad ze třídy polovu-Heuslerových materiálů. Topological insulators (TIs) are exciting materials, which exhibit unprecedented properties, such as helical spinmomentum locking, which leads to large torques for magnetic switching and highly efficient spin current detection. Here we explore the compound YPtBi, an example from the class of half-Heusler materials, for which the typical band inversion of topological insulators was predicted. We prepared this material as thin films by conventional cosputtering from elementary targets. By in situ time-of-flight mo…

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

Journal of physics / Condensed matter 29(25), 255001 - (2017). doi:10.1088/1361-648X/aa7173

Compact setup for spin-, time-, and angle-resolved photoemission spectroscopy.

Review of scientific instruments 91(6), 063001 (2020). doi:10.1063/5.0004861

Investigation of Many‐Body Effects in the Quasi‐Two‐Dimensional Electronic System of Organic Charge‐Transfer Salts

Theoretical study of new acceptor and donor molecules based on polycyclic aromatic hydrocarbons

Functionalized polcyclic aromatic hydrocarbons (PAHs) are an interesting class of molecules in which the electronic state of the graphene-like hydrocarbon part is tuned by the functional group. Searching for new types of donor and acceptor molecules, a set of new PAHs has recently been investigated experimentally using ultraviolet photoelectron spectroscopy (UPS). In this work, the electronic structure of the PAHs is studied numerically with the help of B3LYP hybrid density functionals. Using the DELTA-SCF method, electron binding energies have been determined which affirm, specify and complement the UPS data. Symmetry properties of molecular orbitals are analyzed for a categorization and a…

Quantitative spin polarization analysis in photoelectron emission microscopy with an imaging spin filter.

Abstract Using a photoelectron emission microscope (PEEM), we demonstrate spin-resolved electron spectroscopic imaging of ultrathin magnetic Co films grown on Cu(100). The spin-filter, based on the spin-dependent reflection of low energy electrons from a W(100) crystal, is attached to an aberration corrected electrostatic energy analyzer coupled to an electrostatic PEEM column. We present a method for the quantitative measurement of the electron spin polarization at 4×10 3 points of the PEEM image, simultaneously. This approach uses the subsequent acquisition of two images with different scattering energies of the electrons at the W(100) target to directly derive the spin polarization witho…

Hard x-ray photoelectron spectroscopy: a snapshot of the state-of-the-art in 2020

Journal of physics / Condensed matter 33(23), 233001 (1-44) (2021). doi:10.1088/1361-648X/abeacd

Imaging spin filter for electrons based on specular reflection from iridium (001)

Abstract As Stern–Gerlach type spin filters do not work with electrons, spin analysis of electron beams is accomplished by spin-dependent scattering processes based on spin–orbit or exchange interaction. Existing polarimeters are single-channel devices characterized by an inherently low figure of merit (FoM) of typically 10 −4 –10 −3 . This single-channel approach is not compatible with parallel imaging microscopes and also not with modern electron spectrometers that acquire a certain energy and angular interval simultaneously. We present a novel type of polarimeter that can transport a full image by making use of k -parallel conservation in low-energy electron diffraction. We studied specul…

4D texture of circular dichroism in soft-x-ray photoemission from tungsten

Brief treatment and crisis intervention 21(1), 013017 (2019). doi:10.1088/1367-2630/aaf4cd

Beyond the Heisenberg Model: Anisotropic Exchange Interaction between a Cu-Tetraazaporphyrin Monolayer andFe3O4(100)

The exchange coupling of a single spin localized at the central ion of Cu-tetraazaporphyrin on a magnetite(100) surface has been studied using x-ray magnetic circular dichroism (XMCD). Sum rule analysis of the XMCD spectra results in Cu spin and orbital magnetic moments as a function of the applied external field at low temperatures (20 K). The exchange coupling is positive for magnetization direction perpendicular to the surface (ferromagnetic) while it is negative for in-plane magnetization direction (antiferromagnetic). We attribute the anisotropy of the Heisenberg exchange coupling to an orbitally dependent exchange Hamiltonian.

Analyzing the enforcement of a high-spin ground state for a metallacrown single-molecule magnet

We have studied element-selective magnetic properties of the hetero- and homometallic metallacrowns $\mathrm{Cu}{(\mathrm{II})}_{2}[12\ensuremath{-}{\mathrm{MC}}_{YN(Shi)}\ensuremath{-}4]$ ($Y=\text{Cu}$, Fe, in short ${\mathrm{CuCu}}_{4}$ and ${\mathrm{CuFe}}_{4}$). These metallacrowns comprise four Fe or Cu ions surrounding a central Cu ion. Using x-ray magnetic circular dichroism we have probed local symmetries, electronic configuration, orbital and spin magnetic moments of the magnetic ions. The ratio between the Cu and Fe moment of $\ensuremath{-}0.11$ is independent of temperature in the range of 15 K to 90 K. The Cu moment shows antiparallel to the Fe moment. For ${\mathrm{CuCu}}_{4}…

Temperature Dependence of Electronic and Magnetic Properties of (DOEO)<sub>4</sub>[HgBr<sub>4</sub>]·TCE Single Crystals

The temperature dependence of electronic and magnetic properties of the organic charge-transfer salt (DOEO)4[HgBr4]·TCE was investigated using magnetometry. The magnetic susceptibility shows a maximum at 40 K followed by an onset of a pronounced increase at 70 K and a constant behavior above 120 K. Implications on the charge carrier density are discussed. Combining the magnetometry with resistivity and ESR measurements we propose a sequence of insulating, metallic and semiconducting behavior with increasing temperature. Our results indicate that (DOEO)4[HgBr4]·TCE is close to the boundary between an insulating and conducting ground state.

Multidimensional photoemission spectroscopy—the space-charge limit

New journal of physics 20(3), 033004 - (2018). doi:10.1088/1367-2630/aaa262

Anomalous d-like surface resonances on Mo(110) analyzed by time-of-flight momentum microscopy.

The electronic surface states on Mo(110) have been investigated using time-of-flight momentum microscopy with synchrotron radiation (hν=35 eV). This novel angle-resolved photoemission approach yields a simultaneous acquisition of the E-vs-k spectral function in the full surface Brillouin zone and several eV energy interval. (kx,ky,EB)-maps with 3.4 A(-1) diameter reveal a rich structure of d-like surface resonances in the spin-orbit induced partial band gap. Calculations using the one-step model in its density matrix formulation predict an anomalous state with Dirac-like signature and Rashba spin texture crossing the bandgap at Γ¯ and EB=1.2 eV. The experiment shows that the linear dispersi…

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

Time-of-flight momentum microscopy is developed. It enables direct three-dimensional mapping of the topology of the Fermi surface, identification of electron and hole pockets, and quantification of Fermi velocity as a function of wavevector.

Detekcia vektora spinovej polarizácie vo viackanálovej spinovo rozlýšenej fotoemissie za použitia spinového filtra založeného na Ir(001)

Physical review / B 95(10), 104423 (2017). doi:10.1103/PhysRevB.95.104423

High-resolution hard-x-ray photoelectron diffraction in a momentum microscope—the model case of graphite

New journal of physics 21(11), 113031 - (2019). doi:10.1088/1367-2630/ab51fe

Investigation of a Ge nanoparticle film by means of electron stimulated photon emission spectroscopy

Abstract Electron stimulated photon emission spectroscopy was used for the study of the electronic structure of Ge nanoparticles. A nanoparticle film was prepared by thermal deposition on a quartz substrate. Photon emission was stimulated by electron bombardment at energies of several hundred electron volts. Electron field emission from a W-tip was used at tip voltage U t  = 100–600 eV. A spectrometer in combination with a liquid nitrogen cooled charge-coupled device (CCD) camera was used for light detection. Light emission spectra were measured in the energy range 1.18–4.2 eV. They are characterized by features at ∼1.6 and ∼3.1 eV. A comparison with light emission spectra obtained with ano…

Emitter-site specificity of hard x-ray photoelectron Kikuchi-diffraction

New journal of physics 22(10), 103002 (1-13) (2020). doi:10.1088/1367-2630/abb68b

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

Journal of synchrotron radiation 28(6), 1891 - 1908 (2021). doi:10.1107/S1600577521010511