Co-doped Ceria: Tendency towards ferromagnetism driven by oxygen vacancies

We perform an electronic structure study for cerium oxide homogeneously-doped with cobalt impurities, focusing on the role played by oxygen vacancies and structural relaxation. By means of full-potential ab-initio methods, we explore the possibility of ferromagnetism as observed in recent experiments. Our results indicate that oxygen vacancies seem to be crucial for the appearance of a ferromagnetic alignment among Co impurities, obtaining an increasing tendency towards ferromagnetism with growing vacancy concentration. The estimated couplings cannot explain though, the experimentally observed room-temperature ferromagnetism. In this systematic study, we draw relevant conclusions regarding the location of the oxygen vacancies and the magnetic couplings involved. In particular, we find that oxygen vacancies tend to nucleate in the neighborhood of Co impurities and we get a remarkably strong ferromagnetic coupling between Co atoms and the Ce^{3+} neighboring ions. The calculated magnetic moments per cell depend on the degree of reduction which could explain the wide spread in the magnetization values observed in the experiments

Multi-Color Imaging of Magnetic Co/Pt Multilayers

We demonstrate for the first time the realization of a spatial resolved two color, element-specific imaging experiment at the free-electron laser facility FERMI. Coherent imaging using Fourier transform holography was used to achieve direct real space access to the nanometer length scale of magnetic domains of Co/Pt heterostructures via the element-specific magnetic dichroism in the extreme ultraviolet spectral range. As a first step to implement this technique for studies of ultrafast phenomena we present the spatially resolved response of magnetic domains upon femtosecond laser excitation

Structural dynamics during laser induced ultrafast demagnetization

The mechanism underlying femtosecond laser pulse induced ultrafast magnetization dynamics remains elusive despite two decades of intense research on this phenomenon. Most experiments focused so far on characterizing magnetization and charge carrier dynamics, while first direct measurements of structural dynamics during ultrafast demagnetization were reported only very recently. We here present our investigation of the infrared laser pulse induced ultrafast demagnetization process in a thin Ni film, which characterizes simultaneously magnetization and structural dynamics. This is achieved by employing femtosecond time resolved X-ray resonant magnetic reflectivity (tr-XRMR) as probe technique. The experimental results reveal unambiguously that the sub-picosecond magnetization quenching is accompanied by strong changes in non-magnetic X-ray reflectivity. These changes vary with reflection angle and changes up to 30$\%$ have been observed. Modeling the X-ray reflectivity of the investigated thin film, we can reproduce these changes by a variation of the apparent Ni layer thickness of up to 1$\%$. Extending these simulations to larger incidence angles we show that tr-XRMR can be employed to discriminate experimentally between currently discussed models describing the ultrafast demagnetization phenomenon

Transient magnetic gratings on the nanometer scale

Laser-driven non-local electron dynamics in ultrathin magnetic samples on a sub-10 nm length scale is a key process in ultrafast magnetism. However, the experimental access has been challenging due to the nanoscopic and femtosecond nature of such transport processes. Here, we present a scattering-based experiment relying on a laser-induced electro- and magneto-optical grating in a Co/Pd ferromagnetic multilayer as a new technique to investigate non-local magnetization dynamics on nanometer length and femtosecond timescales. We induce a spatially modulated excitation pattern using tailored Al near-field masks with varying periodicities on a nanometer length scale and measure the first four diffraction orders in an x-ray scattering experiment with magnetic circular dichroism contrast at the free-electron laser facility FERMI, Trieste. The design of the periodic excitation mask leads to a strongly enhanced and characteristic transient scattering response allowing for sub-wavelength in-plane sensitivity for magnetic structures. In conjunction with scattering simulations, the experiment allows us to infer that a potential ultrafast lateral expansion of the initially excited regions of the magnetic film mediated by hot-electron transport and spin transport remains confined to below three nanometers

Spin-dependent resonant quantum tunneling between magnetic nanoparticles on a macroscopic length scale

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Macroscopic quantum phenomena are common features observed in superconductors, superfluid helium, and Bose-Einstein condensates. However, most of quantum transport studies are based on a small number of dots and are not in long-range electron transport length scale. Here we show that spin-dependent resonant quantum tunneling is achieved in the macroscopic length scale (a few millimeters) corresponding to an array of up to 10(4) junctions in a series consisting of Co nanoparticles embedded in an oxygen-deficient TiO(2) matrix. This phenomenon is observed by magnetoresistance measurements at 5 K in a Coulomb blockade regime. We further present a model based on resonant spin-polarized quantum tunneling of electrons of Co particles. It occurs through resonant continuous spin-polarized defect band states located near the Fermi level of the defective TiO(2), which acts as a magnetic tunnel barrier. These results might be potentially useful for future designs of spintronic quantum devices.834Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP

Sub 15 fs X ray pump and X ray probe experiment for the study of ultrafast magnetization dynamics in ferromagnetic alloys

In this paper, we present a new setup for the measurement of element specific ultrafast magnetization dynamics in ferromagnetic thin films with a sub 15 fs time resolution. Our experiment relies on a split and delay approach which allows us to fully exploit the shortest X rays pulses delivered by X ray Free Electrons Lasers close to the attosecond range , in an X ray pump X ray probe geometry. The setup performance is demonstrated by measuring the ultrafast elemental response of Ni and Fe during demagnetization of ferromagnetic Ni and Ni80Fe20 Permalloy samples upon resonant excitation at the corresponding absorption edges. The transient demagnetization process is measured in both reflection and transmission geometry using, respectively, the transverse magneto optical Kerr effect T MOKE and the Faraday effect as probing mechanism

Toward ultrafast magnetic depth profiling using time resolved x ray resonant magnetic reflectivity

During the last two decades, a variety of models have been developed to explain the ultrafast quenching of magnetization following femtosecond optical excitation. These models can be classified into two broad categories, relying either on a local or a non local transfer of angular momentum. The acquisition of the magnetic depth profiles with femtosecond resolution, using time resolved x ray resonant magnetic reflectivity, can distinguish local and non local effects. Here, we demonstrate the feasibility of this technique in a pump probe geometry using a custom built reflectometer at the FLASH2 free electron laser FEL . Although FLASH2 is limited to the production of photons with a fundamental wavelength of 4 amp; 8201;nm amp; 8771;310 amp; 8201;eV , we were able to probe close to the Fe L3 edge 706.8 amp; 8201;eV of a magnetic thin film employing the third harmonic of the FEL. Our approach allows us to extract structural and magnetic asymmetry signals revealing two dynamics on different time scales which underpin a non homogeneous loss of magnetization and a significant dilation of 2 amp; 8201; of the layer thickness followed by oscillations. Future analysis of the data will pave the way to a full quantitative description of the transient magnetic depth profile combining femtosecond with nanometer resolution, which will provide further insight into the microscopic mechanisms underlying ultrafast demagnetizatio

Polarization control of isolated high-harmonic pulses

High-harmonic generation driven by femtosecond lasers makes it possible to capture the fastest dynamics in molecules and materials. However, thus far, the shortest isolated attosecond pulses have only been produced with linear polarization, which limits the range of physics that can be explored. Here, we demonstrate robust polarization control of isolated extreme-ultraviolet pulses by exploiting non-collinear high-harmonic generation driven by two counter-rotating few-cycle laser beams. The circularly polarized supercontinuum is produced at a central photon energy of 33 eV with a transform limit of 190 as and a predicted linear chirp of 330 as. By adjusting the ellipticity of the two counter-rotating driving pulses simultaneously, we control the polarization state of isolated extreme-ultraviolet pulses—from circular through elliptical to linear polarization—without sacrificing conversion efficiency. Access to the purely circularly polarized supercontinuum, combined with full helicity and ellipticity control, paves the way towards attosecond metrology of circular dichroism.The experimental work was carried out at National Tsing Hua University, Institute of Photonics Technologies, supported by the Ministry of Science and Technology, Taiwan (grants 105-2112-M-007-030-MY3, 105-2112-M-001-030 and 104-2112-M-007-012-MY3). The concept of isolated circularly polarized attosecond pulses was developed by C.H.-G., D.D.H., M.M.M., C.G.D., H.C.K., A.B. and A.J.-B.. C.H.-G. acknowledges support from the Marie Curie International Outgoing Fellowship within the EU Seventh Framework Programme for Research and Technological Development (2007–2013), under Research Executive Agency grant agreement no. 328334. C.H.-G. and L.P. acknowledge support from Junta de Castilla y León (SA046U16) and the Ministerio de Economía y Competitividad (FIS2013-44174-P, FIS2016-75652-P). C.H.-G. acknowledges support from a 2017 Leonardo Grant for Researchers and Cultural Creators (BBVA Foundation). M.M.M. and H.C.K. acknowledge support from the Department of Energy Basic Energy Sciences (award no. DE-FG02-99ER14982) for the concepts and experimental set-up. For part of the theory, A.B., A.J.-B., C.G.D., M.M.M. and H.C.K. acknowledge support from a Multidisciplinary University Research Initiatives grant from the Air Force Office of Scientific Research (award no. FA9550-16-1-0121). A.J.-B. also acknowledges support from the US National Science Foundation (grant no. PHY-1734006). This work utilized the Janus supercomputer, which is supported by the US National Science Foundation (grant no. CNS-0821794) and the University of Colorado, Boulder. This research made use of the high-performance computing resources of the Castilla y León Supercomputing Center (SCAYLE, www.scayle.es), financed by the European Regional Development Fund (ERDF). J.L.E. acknowledges support from the National Science Foundation Graduate Research Fellowship (DGE-1144083). L.R. acknowledges support from the Ministerio de Educación, Cultura y Deporte (FPU16/02591)

Megahertz-rate ultrafast X-ray scattering and holographic imaging at the European XFEL

The advent of X-ray free-electron lasers (XFELs) has revolutionized fundamental science, from atomic to condensed matter physics, from chemistry to biology, giving researchers access to X-rays with unprecedented brightness, coherence and pulse duration. All XFEL facilities built until recently provided X-ray pulses at a relatively low repetition rate, with limited data statistics. Here, results from the first megahertz-repetition-rate X-ray scattering experiments at the Spectroscopy and Coherent Scattering (SCS) instrument of the European XFEL are presented. The experimental capabilities that the SCS instrument offers, resulting from the operation at megahertz repetition rates and the availability of the novel DSSC 2D imaging detector, are illustrated. Time-resolved magnetic X-ray scattering and holographic imaging experiments in solid state samples were chosen as representative, providing an ideal test-bed for operation at megahertz rates. Our results are relevant and applicable to any other non-destructive XFEL experiments in the soft X-ray range