Education & Certifications

  • PhD, Stanford University, Applied Physics (2007)
  • MS, Stanford University, Applied Physics
  • BSE, University of Michigan, Engineering Physics (2002)

Contact

  • Work
    wschlott@stanford.edu
    University - Staff Department: SLAC National Accelerator Laboratory Position: Lead Scientist
    • 2575 Sand Hill Rd
    • Mailstop 0019
    • Menlo Park,  California  94025 

Additional Info

  • Mail Code: 19
  • Other Names:
    Bill Schlotter

All Publications

  • Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution. Nature communications Higley, D. J., Reid, A. H., Chen, Z., Guyader, L. L., Hellwig, O., Lutman, A. A., Liu, T., Shafer, P., Chase, T., Dakovski, G. L., Mitra, A., Yuan, E., Schlappa, J., Durr, H. A., Schlotter, W. F., Stohr, J. 2019; 10 (1): 5289

    Abstract

    Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L[Formula: see text] edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.

    View details for DOI 10.1038/s41467-019-13272-5

    View details for PubMedID 31754109

  • Ultrafast time-resolved x-ray scattering reveals diffusive charge order dynamics in La2-x Ba x CuO4. Science advances Mitrano, M., Lee, S., Husain, A. A., Delacretaz, L., Zhu, M., de la Pena Munoz, G., Sun, S. X., Joe, Y. I., Reid, A. H., Wandel, S. F., Coslovich, G., Schlotter, W., van Driel, T., Schneeloch, J., Gu, G. D., Hartnoll, S., Goldenfeld, N., Abbamonte, P. 2019; 5 (8): eaax3346

    Abstract

    Charge order is universal among high-T c cuprates, but its relation to superconductivity is unclear. While static order competes with superconductivity, dynamic order may be favorable and even contribute to Cooper pairing. Using time-resolved resonant soft x-ray scattering at a free-electron laser, we show that the charge order in prototypical La2-x Ba x CuO4 exhibits transverse fluctuations at picosecond time scales. These sub-millielectron volt excitations propagate by Brownian-like diffusion and have an energy scale remarkably close to the superconducting T c. At sub-millielectron volt energy scales, the dynamics are governed by universal scaling laws defined by the propagation of topological defects. Our results show that charge order in La2-x Ba x CuO4 exhibits dynamics favorable to the in-plane superconducting tunneling and establish time-resolved x-rays as a means to study excitations at energy scales inaccessible to conventional scattering techniques.

    View details for DOI 10.1126/sciadv.aax3346

    View details for PubMedID 31453340

  • Disentangling Transient Charge Density and Metal-Ligand Covalency in Photoexcited Ferricyanide with Femtosecond Resonant Inelastic Soft X-ray Scattering JOURNAL OF PHYSICAL CHEMISTRY LETTERS Jay, R. M., Norell, J., Eckert, S., Hantschmann, M., Beye, M., Kennedy, B., Quevedo, W., Schlotter, W. F., Dakovski, G. L., Minitti, M. P., Hoffmann, M. C., Mitra, A., Moeller, S. P., Nordlund, D., Zhang, W., Liang, H. W., Kunnus, K., Kubicek, K., Techert, S. A., Lundberg, M., Wernet, P., Gaffney, K., Odelius, M., Foehlisch, A. 2018; 9 (12): 3538–43

    Abstract

    Soft X-ray spectroscopies are ideal probes of the local valence electronic structure of photocatalytically active metal sites. Here, we apply the selectivity of time-resolved resonant inelastic X-ray scattering at the iron L-edge to the transient charge distribution of an optically excited charge-transfer state in aqueous ferricyanide. Through comparison to steady-state spectra and quantum chemical calculations, the coupled effects of valence-shell closing and ligand-hole creation are experimentally and theoretically disentangled and described in terms of orbital occupancy, metal-ligand covalency, and ligand field splitting, thereby extending established steady-state concepts to the excited-state domain. π-Back-donation is found to be mainly determined by the metal site occupation, whereas the ligand hole instead influences σ-donation. Our results demonstrate how ultrafast resonant inelastic X-ray scattering can help characterize local charge distributions around catalytic metal centers in short-lived charge-transfer excited states, as a step toward future rationalization and tailoring of photocatalytic capabilities of transition-metal complexes.

    View details for PubMedID 29888918

  • LCLS in-photon out: fluorescence measurement of neon using soft x-rays JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS Obaid, R., Buth, C., Dakovski, G. L., Beerwerth, R., Holmes, M., Aldrich, J., Lin, M., Minitti, M., Osipov, T., Schlotter, W., Cederbaum, L. S., Fritzsche, S., Berrah, N. 2018; 51 (3)

    View details for DOI 10.1088/1361-6455/aaa189

    View details for Web of Science ID 000419798400001

  • A novel method for resonant inelastic soft X-ray scattering via photoelectron spectroscopy detection JOURNAL OF SYNCHROTRON RADIATION Dakovski, G. L., Lin, M., Damiani, D. S., Schlotter, W. F., Turner, J. J., Nordlund, D., Ogasawara, H. 2017; 24: 1180–86

    Abstract

    A method for measuring resonant inelastic X-ray scattering based on the conversion of X-ray photons into photoelectrons is presented. The setup is compact, relies on commercially available detectors, and offers significant flexibility. This method is demonstrated at the Linac Coherent Light Source with ∼0.5 eV resolution at the cobalt L3-edge, with signal rates comparable with traditional grating spectrometers.

    View details for PubMedID 29091061

  • Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Eckert, S., Norell, J., Miedema, P. S., Beye, M., Fondell, M., Quevedo, W., Kennedy, B., Hantschmann, M., Pietzsch, A., Van Kuiken, B. E., Ross, M., Minitti, M. P., Moeller, S. P., Schlotter, W. F., Khalil, M., Odelius, M., Foehlisch, A. 2017; 56 (22): 6088–92

    Abstract

    The femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort timescale.

    View details for PubMedID 28374523

    View details for PubMedCentralID PMC5485001

  • Magnetic Switching in Granular FePt Layers Promoted by Near-Field Laser Enhancement NANO LETTERS Granitzka, P. W., Jal, E., Le Guyader, L., Savoini, M., Higley, D. J., Liu, T., Chen, Z., Chase, T., Ohldag, H., Dakovski, G. L., Schlotter, W. F., Carron, S., Hoffman, M. C., Gray, A. X., Shafer, P., Arenholz, E., Hellwig, O., Mehta, V., Takahashi, Y. K., Wang, J., Fullerton, E. E., Stoehr, J., Reid, A. H., Duerr, H. A. 2017; 17 (4): 2426-2432

    Abstract

    Light-matter interaction at the nanoscale in magnetic materials is a topic of intense research in view of potential applications in next-generation high-density magnetic recording. Laser-assisted switching provides a pathway for overcoming the material constraints of high-anisotropy and high-packing density media, though much about the dynamics of the switching process remains unexplored. We use ultrafast small-angle X-ray scattering at an X-ray free-electron laser to probe the magnetic switching dynamics of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. We observe that the combination of laser excitation and applied static magnetic field, 1 order of magnitude smaller than the coercive field, can overcome the magnetic anisotropy barrier between "up" and "down" magnetization, enabling magnetization switching. This magnetic switching is found to be inhomogeneous throughout the material with some individual FePt nanoparticles neither switching nor demagnetizing. The origin of this behavior is identified as the near-field modification of the incident laser radiation around FePt nanoparticles. The fraction of not-switching nanoparticles is influenced by the heat flow between FePt and a heat-sink layer.

    View details for DOI 10.1021/acs.nanolett.7b00052

    View details for Web of Science ID 000399354500047

    View details for PubMedID 28272897

  • Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics NEW JOURNAL OF PHYSICS Kunnus, K., Josefsson, I., Rajkovic, I., Schreck, S., Quevedo, W., Beye, M., Greubel, S., Scholz, M., Nordlund, D., Zhang, W., Hartsock, R. W., Gaffney, K. J., Schlotter, W. F., Turner, J. J., Kennedy, B., Hennies, F., Techert, S., Wernet, P., Odelius, M., Foehlisch, A. 2016; 18

    View details for DOI 10.1088/1367-2630/18/10/103011

    View details for Web of Science ID 000386047000005

  • Chemical Bond Activation Observed with an X-ray Laser JOURNAL OF PHYSICAL CHEMISTRY LETTERS Beye, M., Oberg, H., Xin, H., Dakovski, G. L., Dell'Angela, M., Foehlisch, A., Gladh, J., Hantschmann, M., Hieke, F., Kaya, S., Kuehn, D., LaRue, J., Mercurio, G., Minitti, M. P., Mitra, A., Moeller, S. P., Ng, M. L., Nilsson, A., Nordlund, D., Norskov, J., Ostrom, H., Ogasawara, H., Persson, M., Schlotter, W. F., Sellberg, J. A., Wolf, M., Abild-Pedersen, F., Pettersson, L. G., Wurth, W. 2016; 7 (18): 3647-3651

    Abstract

    The concept of bonding and antibonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Here we apply time-resolved soft X-ray spectroscopy at a free-electron laser to directly observe the decreased bonding-antibonding splitting following bond-activation using an ultrashort optical laser pulse.

    View details for DOI 10.1021/acs.jpclett.6b01543

    View details for Web of Science ID 000383641800019

  • Chemical Bond Activation Observed with an X-ray Laser. journal of physical chemistry letters Beye, M., Öberg, H., Xin, H., Dakovski, G. L., Dell'Angela, M., Föhlisch, A., Gladh, J., Hantschmann, M., Hieke, F., Kaya, S., Kühn, D., LaRue, J., Mercurio, G., Minitti, M. P., Mitra, A., Moeller, S. P., Ng, M. L., Nilsson, A., Nordlund, D., Nørskov, J., Öström, H., Ogasawara, H., Persson, M., Schlotter, W. F., Sellberg, J. A., Wolf, M., Abild-Pedersen, F., Pettersson, L. G., Wurth, W. 2016; 7 (18): 3647-3651

    Abstract

    The concept of bonding and antibonding orbitals is fundamental in chemistry. The population of those orbitals and the energetic difference between the two reflect the strength of the bonding interaction. Weakening the bond is expected to reduce this energetic splitting, but the transient character of bond-activation has so far prohibited direct experimental access. Here we apply time-resolved soft X-ray spectroscopy at a free-electron laser to directly observe the decreased bonding-antibonding splitting following bond-activation using an ultrashort optical laser pulse.

    View details for DOI 10.1021/acs.jpclett.6b01543

    View details for PubMedID 27584914

  • Polarization control in an X-ray free-electron laser NATURE PHOTONICS Lutman, A. A., MacArthur, J. P., Ilchen, M., Lindahl, A. O., Buck, J., Coffee, R. N., Dakovski, G. L., Dammann, L., Ding, Y., Durr, H. A., Glaser, L., Grunert, J., Hartmann, G., Hartmann, N., Higley, D., Hirsch, K., Levashov, Y. I., Marinelli, A., Maxwell, T., Mitra, A., Moeller, S., Osipov, T., Peters, F., Planas, M., Shevchuk, I., Schlotter, W. F., Scholz, F., Seltmann, J., Viefhaus, J., Walter, P., Wolf, Z. R., Huang, Z., Nuhn, H. 2016; 10 (7): 468-472

    View details for DOI 10.1038/NPHOTON.2016.79

    View details for Web of Science ID 000378839600013

  • Linac Coherent Light Source: The first five years REVIEWS OF MODERN PHYSICS Bostedt, C., Boutet, S., Fritz, D. M., Huang, Z., Lee, H. J., Lemke, H. T., Robert, A., Schlotter, W. F., Turner, J. J., Williams, G. J. 2016; 88 (1)

    View details for DOI 10.1103/RevModPhys.88.015007

    View details for Web of Science ID 000371723300002

  • Femtosecond X-ray magnetic circular dichroism absorption spectroscopy at an X-ray free electron laser REVIEW OF SCIENTIFIC INSTRUMENTS Higley, D. J., Hirsch, K., Dakovski, G. L., Jal, E., Yuan, E., Liu, T., Lutman, A. A., MacArthur, J. P., Arenholz, E., Chen, Z., Coslovich, G., Denes, P., Granitzka, P. W., Hart, P., Hoffmann, M. C., Joseph, J., Le Guyader, L., Mitra, A., Moeller, S., Ohldag, H., Seaberg, M., Shafer, P., Stoehr, J., Tsukamoto, A., Nuhn, H., Reid, A. H., Duerr, H. A., Schlotter, W. F. 2016; 87 (3)

    Abstract

    X-ray magnetic circular dichroism spectroscopy using an X-ray free electron laser is demonstrated with spectra over the Fe L(3,2)-edges. The high brightness of the X-ray free electron laser combined with high accuracy detection of incident and transmitted X-rays enables ultrafast X-ray magnetic circular dichroism studies of unprecedented sensitivity. This new capability is applied to a study of all-optical magnetic switching dynamics of Fe and Gd magnetic sublattices in a GdFeCo thin film above its magnetization compensation temperature.

    View details for DOI 10.1063/1.4944410

    View details for Web of Science ID 000373713300011

    View details for PubMedID 27036761

  • Combining THz laser excitation with resonant soft X-ray scattering at the Linac Coherent Light Source JOURNAL OF SYNCHROTRON RADIATION Turner, J. J., Dakovski, G. L., Hoffmann, M. C., Hwang, H. Y., Zarem, A., Schlotter, W. F., Moeller, S., Minitti, M. P., Staub, U., Johnson, S., Mitra, A., Swiggers, M., Noonan, P., Curiel, G. I., Holmes, M. 2015; 22: 621-625

    Abstract

    This paper describes the development of new instrumentation at the Linac Coherent Light Source for conducting THz excitation experiments in an ultra high vacuum environment probed by soft X-ray diffraction. This consists of a cantilevered, fully motorized mirror system which can provide 600 kV cm(-1) electric field strengths across the sample and an X-ray detector that can span the full Ewald sphere with in-vacuum motion. The scientific applications motivated by this development, the details of the instrument, and spectra demonstrating the field strengths achieved using this newly developed system are discussed.

    View details for DOI 10.1107/S1600577515005998

    View details for Web of Science ID 000353920300024

    View details for PubMedID 25931077

    View details for PubMedCentralID PMC4416678

  • Pulse energy measurement at the SXR instrument JOURNAL OF SYNCHROTRON RADIATION Moeller, S., Brown, G., Dakovski, G., Hill, B., Holmes, M., Loos, J., Maida, R., Paiser, E., Schlotter, W., Turner, J. J., Wallace, A., Jastrow, U., Kreis, S., Sorokin, A. A., Tiedtke, K. 2015; 22: 606–11

    Abstract

    A gas monitor detector was implemented and characterized at the Soft X-ray Research (SXR) instrument to measure the average, absolute and pulse-resolved photon flux of the LCLS beam in the energy range between 280 and 2000 eV. The detector is placed after the monochromator and addresses the need to provide reliable absolute pulse energy as well as pulse-resolved measurements for the various experiments at this instrument. This detector provides a reliable non-invasive measurement for determining flux levels on the samples in the downstream experimental chamber and for optimizing signal levels of secondary detectors and for the essential need of data normalization. The design, integration into the instrument and operation are described, and examples of its performance are given.

    View details for PubMedID 25931075

    View details for PubMedCentralID PMC4416676

  • The Soft X-ray Research instrument at the Linac Coherent Light Source JOURNAL OF SYNCHROTRON RADIATION Dakovski, G. L., Heimann, P., Holmes, M., Krupin, O., Minitti, M. P., Mitra, A., Moeller, S., Rowen, M., Schlotter, W. F., Turner, J. J. 2015; 22: 498–502

    Abstract

    The Soft X-ray Research instrument provides intense ultrashort X-ray pulses in the energy range 280-2000 eV. A diverse set of experimental stations may be installed to investigate a broad range of scientific topics such as ultrafast chemistry, highly correlated materials, magnetism, surface science, and matter under extreme conditions. A brief description of the main instrument components will be given, followed by some selected scientific highlights.

    View details for PubMedID 25931059

    View details for PubMedCentralID PMC4416666

  • Irreversible transformation of ferromagnetic ordered stripe domains in single-shot infrared-pump/resonant-x-ray-scattering-probe experiments PHYSICAL REVIEW B Bergeard, N., Schaffert, S., Lopez-Flores, V., Jaouen, N., Geilhufe, J., Guenther, C. M., Schneider, M., Graves, C., Wang, T., Wu, B., Scherz, A., Baumier, C., Delaunay, R., Fortuna, F., Tortarolo, M., Tudu, B., Krupin, O., Minitti, M. P., Robinson, J., Schlotter, W. F., Turner, J. J., Luening, J., Eisebitt, S., Boeglin, C. 2015; 91 (5)

    View details for DOI 10.1103/PhysRevB.91.054416

    View details for Web of Science ID 000351770800003

  • X-ray emission spectroscopy of bulk liquid water in "no-man's land". journal of chemical physics Sellberg, J. A., McQueen, T. A., Laksmono, H., Schreck, S., Beye, M., Deponte, D. P., Kennedy, B., Nordlund, D., Sierra, R. G., Schlesinger, D., Tokushima, T., Zhovtobriukh, I., Eckert, S., Segtnan, V. H., Ogasawara, H., Kubicek, K., Techert, S., Bergmann, U., Dakovski, G. L., Schlotter, W. F., Harada, Y., Bogan, M. J., Wernet, P., Föhlisch, A., Pettersson, L. G., Nilsson, A. 2015; 142 (4): 044505-?

    Abstract

    The structure of bulk liquid water was recently probed by x-ray scattering below the temperature limit of homogeneous nucleation (TH) of ∼232 K [J. A. Sellberg et al., Nature 510, 381-384 (2014)]. Here, we utilize a similar approach to study the structure of bulk liquid water below TH using oxygen K-edge x-ray emission spectroscopy (XES). Based on previous XES experiments [T. Tokushima et al., Chem. Phys. Lett. 460, 387-400 (2008)] at higher temperatures, we expected the ratio of the 1b1' and 1b1″ peaks associated with the lone-pair orbital in water to change strongly upon deep supercooling as the coordination of the hydrogen (H-) bonds becomes tetrahedral. In contrast, we observed only minor changes in the lone-pair spectral region, challenging an interpretation in terms of two interconverting species. A number of alternative hypotheses to explain the results are put forward and discussed. Although the spectra can be explained by various contributions from these hypotheses, we here emphasize the interpretation that the line shape of each component changes dramatically when approaching lower temperatures, where, in particular, the peak assigned to the proposed disordered component would become more symmetrical as vibrational interference becomes more important.

    View details for DOI 10.1063/1.4905603

    View details for PubMedID 25637993

  • Reabsorption of soft x-ray emission at high x-ray free-electron laser fluences. Physical review letters Schreck, S., Beye, M., Sellberg, J. A., McQueen, T., Laksmono, H., Kennedy, B., Eckert, S., Schlesinger, D., Nordlund, D., Ogasawara, H., Sierra, R. G., Segtnan, V. H., Kubicek, K., Schlotter, W. F., Dakovski, G. L., Moeller, S. P., Bergmann, U., Techert, S., Pettersson, L. G., Wernet, P., Bogan, M. J., Harada, Y., Nilsson, A., Föhlisch, A. 2014; 113 (15): 153002-?

    Abstract

    We report on oxygen K-edge soft x-ray emission spectroscopy from a liquid water jet at the Linac Coherent Light Source. We observe significant changes in the spectral content when tuning over a wide range of incident x-ray fluences. In addition the total emission yield decreases at high fluences. These modifications result from reabsorption of x-ray emission by valence-excited molecules generated by the Auger cascade. Our observations have major implications for future x-ray emission studies at intense x-ray sources. We highlight the importance of the x-ray pulse length with respect to the core-hole lifetime.

    View details for PubMedID 25375708

  • Reabsorption of Soft X-Ray Emission at High X-Ray Free-Electron Laser Fluences PHYSICAL REVIEW LETTERS Schreck, S., Beye, M., Sellberg, J. A., McQueen, T., Laksmono, H., Kennedy, B., Eckert, S., Schlesinger, D., Nordlund, D., Ogasawara, H., Sierra, R. G., Segtnan, V. H., Kubicek, K., Schlotter, W. F., Dakovski, G. L., Moeller, S. P., Bergmann, U., Techert, S., Pettersson, L. G., Wernet, P., Bogan, M. J., Harada, Y., Nilsson, A., Foehlisch, A. 2014; 113 (15)

    Abstract

    We report on oxygen K-edge soft x-ray emission spectroscopy from a liquid water jet at the Linac Coherent Light Source. We observe significant changes in the spectral content when tuning over a wide range of incident x-ray fluences. In addition the total emission yield decreases at high fluences. These modifications result from reabsorption of x-ray emission by valence-excited molecules generated by the Auger cascade. Our observations have major implications for future x-ray emission studies at intense x-ray sources. We highlight the importance of the x-ray pulse length with respect to the core-hole lifetime.

    View details for DOI 10.1103/PhysRevLett.113.153002

    View details for Web of Science ID 000344245600005

  • Atomic-Scale Perspective of Ultrafast Charge Transfer at a Dye-Semiconductor Interface JOURNAL OF PHYSICAL CHEMISTRY LETTERS Siefermann, K. R., Pemmaraju, C. D., Neppl, S., Shavorskiy, A., Cordones, A. A., Vura-Weis, J., Slaughter, D. S., Sturm, F. P., Weise, F., Bluhm, H., Strader, M. L., Cho, H., Lin, M., Bacellar, C., Khurmi, C., Guo, J., Coslovich, G., Robinson, J. S., Kaindl, R. A., Schoenlein, R. W., Belkacem, A., Neumark, D. M., Leone, S. R., Nordlund, D., Ogasawara, H., Krupin, O., Turner, J. J., Schlotter, W. F., Holmes, M. R., Messerschmidt, M., Minitti, M. P., Gul, S., Zhang, J. Z., Huse, N., Prendergast, D., Gessner, O. 2014; 5 (15): 2753-2759

    Abstract

    Understanding interfacial charge-transfer processes on the atomic level is crucial to support the rational design of energy-challenge relevant systems such as solar cells, batteries, and photocatalysts. A femtosecond time-resolved core-level photoelectron spectroscopy study is performed that probes the electronic structure of the interface between ruthenium-based N3 dye molecules and ZnO nanocrystals within the first picosecond after photoexcitation and from the unique perspective of the Ru reporter atom at the center of the dye. A transient chemical shift of the Ru 3d inner-shell photolines by (2.3 ± 0.2) eV to higher binding energies is observed 500 fs after photoexcitation of the dye. The experimental results are interpreted with the aid of ab initio calculations using constrained density functional theory. Strong indications for the formation of an interfacial charge-transfer state are presented, providing direct insight into a transient electronic configuration that may limit the efficiency of photoinduced free charge-carrier generation.

    View details for DOI 10.1021/jz501264x

    View details for Web of Science ID 000340222200044

    View details for PubMedID 26277975

  • L-Edge X-ray Absorption Spectroscopy of Dilute Systems Relevant to Metalloproteins Using an X-ray Free-Electron Laser JOURNAL OF PHYSICAL CHEMISTRY LETTERS Mitzner, R., Rehanek, J., Kern, J., Gul, S., Hattne, J., Taguchi, T., Alonso-Mori, R., Tran, R., Weniger, C., Schroeder, H., Quevedo, W., Laksmono, H., Sierra, R. G., Han, G., Lassalle-Kaiser, B., Koroidov, S., Kubicek, K., Schreck, S., Kunnus, K., Brzhezinskaya, M., Firsov, A., Minitti, M. P., Turner, J. J., Moeller, S., Sauter, N. K., Bogan, M. J., Nordlund, D., Schlotter, W. F., Messinger, J., Borovik, A., Techert, S., de Groot, F. M., Foehlisch, A., Erko, A., Bergmann, U., Yachandra, V. K., Wernet, P., Yano, J. 2013; 4 (21): 3641-3647

    Abstract

    L-edge spectroscopy of 3d transition metals provides important electronic structure information and has been used in many fields. However, the use of this method for studying dilute aqueous systems, such as metalloenzymes, has not been prevalent because of severe radiation damage and the lack of suitable detection systems. Here we present spectra from a dilute Mn aqueous solution using a high-transmission zone-plate spectrometer at the Linac Coherent Light Source (LCLS). The spectrometer has been optimized for discriminating the Mn L-edge signal from the overwhelming O K-edge background that arises from water and protein itself, and the ultrashort LCLS X-ray pulses can outrun X-ray induced damage. We show that the deviations of the partial-fluorescence yield-detected spectra from the true absorption can be well modeled using the state-dependence of the fluorescence yield, and discuss implications for the application of our concept to biological samples.

    View details for DOI 10.1021/jz401837f

    View details for Web of Science ID 000326845200010

    View details for PubMedCentralID PMC3901369

  • L-Edge X-ray Absorption Spectroscopy of Dilute Systems Relevant to Metalloproteins Using an X-ray Free-Electron Laser. The journal of physical chemistry letters Mitzner, R., Rehanek, J., Kern, J., Gul, S., Hattne, J., Taguchi, T., Alonso-Mori, R., Tran, R., Weniger, C., Schröder, H., Quevedo, W., Laksmono, H., Sierra, R. G., Han, G., Lassalle-Kaiser, B., Koroidov, S., Kubicek, K., Schreck, S., Kunnus, K., Brzhezinskaya, M., Firsov, A., Minitti, M. P., Turner, J. J., Moeller, S., Sauter, N. K., Bogan, M. J., Nordlund, D., Schlotter, W. F., Messinger, J., Borovik, A., Techert, S., de Groot, F. M., Föhlisch, A., Erko, A., Bergmann, U., Yachandra, V. K., Wernet, P., Yano, J. 2013; 4 (21): 3641-3647

    Abstract

    L-edge spectroscopy of 3d transition metals provides important electronic structure information and has been used in many fields. However, the use of this method for studying dilute aqueous systems, such as metalloenzymes, has not been prevalent because of severe radiation damage and the lack of suitable detection systems. Here we present spectra from a dilute Mn aqueous solution using a high-transmission zone-plate spectrometer at the Linac Coherent Light Source (LCLS). The spectrometer has been optimized for discriminating the Mn L-edge signal from the overwhelming O K-edge background that arises from water and protein itself, and the ultrashort LCLS X-ray pulses can outrun X-ray induced damage. We show that the deviations of the partial-fluorescence yield-detected spectra from the true absorption can be well modeled using the state-dependence of the fluorescence yield, and discuss implications for the application of our concept to biological samples.

    View details for DOI 10.1021/jz401837f

    View details for PubMedID 24466387

    View details for PubMedCentralID PMC3901369

  • Time-Resolved X-Ray Photoelectron Spectroscopy Techniques For Real-Time Studies Of Interfacial Charge Transfer Dynamics 22nd International Conference on the Application of Accelerators in Research and Industry (CAARI) Shavorskiy, A., Cordones, A., Vura-Weis, J., Siefermann, K., Slaughter, D., Sturm, F., Weise, F., Bluhm, H., Strader, M., Cho, H., Lin, M., Bacellar, C., Khurmi, C., Hertlein, M., Guo, J., Tyliszczak, T., Prendergast, D., Coslovich, G., Robinson, J., Kaindl, R. A., Schoenlein, R. W., Belkacem, A., Weber, T., Neumark, D. M., Leone, S. R., Nordlund, D., Ogasawara, H., Nilsson, A. R., Krupin, O., Turner, J. J., Schlotter, W. F., Holmes, M. R., Heimann, P. A., Messerschmidt, M., Minitti, M. P., Beye, M., Gul, S., Zhang, J. Z., Huse, N., Gessner, O. AMER INST PHYSICS. 2013: 475–479

    View details for DOI 10.1063/1.4802374

    View details for Web of Science ID 000319997900095

  • Development, experimental performance and damage properties of x-ray optics for the LCLS free-electron laser Soufli, R., Fernandez-Perea, M., Krzywinski, J., Rich, D. W., Baker, S. L., Robinson, J. C., Hau-Riege, S., Gullikson, E. M., Yashchuk, V. V., McKinney, W. R., Heimann, P., Schlotter, W. F., Rowen, M., Montanez, P. A., Boutet, S., Juha, L., Bajt, S., London, R., Hudec, R., Pina, L. SPIE-INT SOC OPTICAL ENGINEERING. 2013

    View details for DOI 10.1117/12.2019197

    View details for Web of Science ID 000329577700001

  • A setup for resonant inelastic soft x-ray scattering on liquids at free electron laser light sources REVIEW OF SCIENTIFIC INSTRUMENTS Kunnus, K., Rajkovic, I., Schreck, S., Quevedo, W., Eckert, S., Beye, M., Suljoti, E., Weniger, C., Kalus, C., Gruebel, S., Scholz, M., Nordlund, D., Zhang, W., Hartsock, R. W., Gaffney, K. J., Schlotter, W. F., Turner, J. J., Kennedy, B., Hennies, F., Techert, S., Wernet, P., Foehlisch, A. 2012; 83 (12)

    Abstract

    We present a flexible and compact experimental setup that combines an in vacuum liquid jet with an x-ray emission spectrometer to enable static and femtosecond time-resolved resonant inelastic soft x-ray scattering (RIXS) measurements from liquids at free electron laser (FEL) light sources. We demonstrate the feasibility of this type of experiments with the measurements performed at the Linac Coherent Light Source FEL facility. At the FEL we observed changes in the RIXS spectra at high peak fluences which currently sets a limit to maximum attainable count rate at FELs. The setup presented here opens up new possibilities to study the structure and dynamics in liquids.

    View details for DOI 10.1063/1.4772685

    View details for Web of Science ID 000312834300010

    View details for PubMedID 23277974

  • Femtosecond Single-Shot Imaging of Nanoscale Ferromagnetic Order in Co/Pd Multilayers Using Resonant X-Ray Holography PHYSICAL REVIEW LETTERS Wang, T., Zhu, D., Wu, B., Graves, C., Schaffert, S., Rander, T., Mueller, L., Vodungbo, B., Baumier, C., Bernstein, D. P., Braeuer, B., Cros, V., de Jong, S., Delaunay, R., Fognini, A., Kukreja, R., Lee, S., Lopez-Flores, V., Mohanty, J., Pfau, B., Popescu, H., Sacchi, M., Sardinha, A. B., Sirotti, F., Zeitoun, P., Messerschmidt, M., Turner, J. J., Schlotter, W. F., Hellwig, O., Mattana, R., Jaouen, N., Fortuna, F., Acremann, Y., Gutt, C., Duerr, H. A., Beaurepaire, E., Boeglin, C., Eisebitt, S., Gruebel, G., Luening, J., Stoehr, J., Scherz, A. O. 2012; 108 (26)

    Abstract

    We present the first single-shot images of ferromagnetic, nanoscale spin order taken with femtosecond x-ray pulses. X-ray-induced electron and spin dynamics can be outrun with pulses shorter than 80 fs in the investigated fluence regime, and no permanent aftereffects in the samples are observed below a fluence of 25 mJ/cm(2). Employing resonant spatially muliplexed x-ray holography results in a low imaging threshold of 5 mJ/cm(2). Our results open new ways to combine ultrafast laser spectroscopy with sequential snapshot imaging on a single sample, generating a movie of excited state dynamics.

    View details for DOI 10.1103/PhysRevLett.108.267403

    View details for PubMedID 23005013

  • Development and calibration of mirrors and gratings for the soft x-ray materials science beamline at the Linac Coherent Light Source free-electron laser APPLIED OPTICS Soufli, R., Fernandez-Perea, M., Baker, S. L., Robinson, J. C., Gullikson, E. M., Heimann, P., Yashchuk, V. V., McKinney, W. R., Schlotter, W. F., Rowen, M. 2012; 51 (12): 2118–28

    Abstract

    This work discusses the development and calibration of the x-ray reflective and diffractive elements for the Soft X-ray Materials Science (SXR) beamline of the Linac Coherent Light Source (LCLS) free-electron laser (FEL), designed for operation in the 500 to 2000 eV region. The surface topography of three Si mirror substrates and two Si diffraction grating substrates was examined by atomic force microscopy (AFM) and optical profilometry. The figure of the mirror substrates was also verified via surface slope measurements with a long trace profiler. A boron carbide (B4C) coating especially optimized for the LCLS FEL conditions was deposited on all SXR mirrors and gratings. Coating thickness uniformity of 0.14 nm root mean square (rms) across clear apertures extending to 205 mm length was demonstrated for all elements, as required to preserve the coherent wavefront of the LCLS source. The reflective performance of the mirrors and the diffraction efficiency of the gratings were calibrated at beamline 6.3.2 at the Advanced Light Source synchrotron. To verify the integrity of the nanometer-scale grating structure, the grating topography was examined by AFM before and after coating. This is to our knowledge the first time B4C-coated diffraction gratings are demonstrated for operation in the soft x-ray region.

    View details for DOI 10.1364/AO.51.002118

    View details for Web of Science ID 000303262200039

    View details for PubMedID 22534924

  • Ultrahigh 22 nm resolution coherent diffractive imaging using a desktop 13 nm high harmonic source OPTICS EXPRESS Seaberg, M. D., Adams, D. E., Townsend, E. L., Raymondson, D. A., Schlotter, W. F., Liu, Y., Menoni, C. S., Rong, L., Chen, C., Miao, J., Kapteyn, H. C., Murnane, M. M. 2011; 19 (23): 22470–79

    Abstract

    New diffractive imaging techniques using coherent x-ray beams have made possible nanometer-scale resolution imaging by replacing the optics in a microscope with an iterative phase retrieval algorithm. However, to date very high resolution imaging (< 40 nm) was limited to large-scale synchrotron facilities. Here, we present a significant advance in image resolution and capabilities for desktop soft x-ray microscopes that will enable widespread applications in nanoscience and nanotechnology. Using 13 nm high harmonic beams, we demonstrate a record 22 nm spatial resolution for any tabletop x-ray microscope. Finally, we show that unique information about the sample can be obtained by extracting 3-D information at very high numerical apertures.

    View details for DOI 10.1364/OE.19.022470

    View details for Web of Science ID 000296904700027

    View details for PubMedID 22109124

  • Linac Coherent Light Source soft x-ray materials science instrument optical design and monochromator commissioning REVIEW OF SCIENTIFIC INSTRUMENTS Heimann, P., Krupin, O., Schlotter, W. F., Turner, J., Krzywinski, J., Sorgenfrei, F., Messerschmidt, M., Bernstein, D., Chalupsky, J., Hajkova, V., Hau-Riege, S., Holmes, M., Juha, L., Kelez, N., Luening, J., Nordlund, D., Fernandez Perea, M., Scherz, A., Soufli, R., Wurth, W., Rowen, M. 2011; 82 (9): 093104

    Abstract

    We present the x-ray optical design of the soft x-ray materials science instrument at the Linac Coherent Light Source, consisting of a varied line-spaced grating monochromator and Kirkpatrick-Baez refocusing optics. Results from the commissioning of the monochromator are shown. A resolving power of 3000 was achieved, which is within a factor of two of the design goal.

    View details for DOI 10.1063/1.3633947

    View details for Web of Science ID 000295621100005

    View details for PubMedID 21974570

  • Ultrafast dynamics in the bonding orbitals while CO desorbs from a Ru surface Anniyev, T., Beye, M., Coffee, R., Dell'Angela, M., Foehlisch, A., Gladh, J., Katayama, T., Kaya, S., Krupin, O., Nilsson, A. R., Nordlund, D., Ogasawara, H., Ostrom, H., Schlotter, W. F., Sellberg, J. A., Sorgenfrei, F., Turner, J. J., Wolf, M., Wurth, W. AMER CHEMICAL SOC. 2011

    View details for Web of Science ID 000291982803920

  • Ultrafast core level shifts in a laser excited oxygen-covered Ru surface Anniyev, T., Beye, M., Coffee, R., Dell'Angela, M., Foehlisch, A., Gladh, J., Katayama, T., Kaya, S., Krupin, O., Nilsson, A. R., Nordlund, D., Ogasawara, H., Ostrom, H., Schlotter, W. F., Sellberg, J. A., Sorgenfrei, F., Turner, J. J., Wolf, M., Wurth, W. AMER CHEMICAL SOC. 2011

    View details for Web of Science ID 000291982803944

  • Sub-30nm Spatial Resolution Imaging Using a Tabletop 13nm High Harmonic Seaberg, M. D., Adams, D. E., Schlotter, W. F., Liu, Y., Menoni, C., Murnane, M., Kapteyn, H., IEEE IEEE. 2011

    View details for Web of Science ID 000295612402037

  • The liquid-liquid phase transition in silicon revealed by snapshots of valence electrons. Proceedings of the National Academy of Sciences of the United States of America Beye, M., Sorgenfrei, F., Schlotter, W. F., Wurth, W., Föhlisch, A. 2010; 107 (39): 16772-6

    Abstract

    The basis for the anomalies of water is still mysterious. Quite generally tetrahedrally coordinated systems, also silicon, show similar thermodynamic behavior but lack--like water--a thorough explanation. Proposed models--controversially discussed--explain the anomalies as a remainder of a first-order phase transition between high and low density liquid phases, buried deeply in the "no man's land"--a part of the supercooled liquid region where rapid crystallization prohibits any experimental access. Other explanations doubt the existence of the phase transition and its first-order nature. Here, we provide experimental evidence for the first-order-phase transition in silicon. With ultrashort optical pulses of femtosecond duration we instantaneously heat the electronic system of silicon while the atomic structure as defined by the much heavier nuclear system remains initially unchanged. Only on a picosecond time scale the energy is transferred into the atomic lattice providing the energy to drive the phase transitions. With femtosecond X-ray pulses from FLASH, the free-electron laser at Hamburg, we follow the evolution of the valence electronic structure during this process. As the relevant phases are easily distinguishable in their electronic structure, we track how silicon melts into the low-density-liquid phase while a second phase transition into the high-density-liquid phase only occurs after the latent heat for the first-order phase transition has been transferred to the atomic structure. Proving the existence of the liquid-liquid phase transition in silicon, the hypothesized liquid-liquid scenario for water is strongly supported.

    View details for DOI 10.1073/pnas.1006499107

    View details for PubMedID 20805512

    View details for PubMedCentralID PMC2947918

  • Magnetic imaging at linearly polarized x-ray sources OPTICS EXPRESS Pfau, B., Guenther, C. M., Koennecke, R., Guehrs, E., Hellwig, O., Schlotter, W. F., Eisebitt, S. 2010; 18 (13): 13608–15

    Abstract

    We present a method for high-resolution magnetic imaging at linearly polarized partially coherent x-ray sources. The magnetic imaging was realized via Fourier transform holography. In order to achieve elliptical x-ray polarization, three different filters were designed based on the x-ray magnetic circular dichroism effect. We present proof-of-principle images of magnetic nanostructures and discuss the application of the method for future experiments at free-electron laser sources.

    View details for DOI 10.1364/OE.18.013608

    View details for Web of Science ID 000279009900035

    View details for PubMedID 20588494

  • Lensless Microscopy and Holography with 60 nm Resolution using Tabletop Coherent Soft X-Rays Raymondson, D. A., Sandberg, R. L., Schlotter, W. F., Raines, K., La-O-Vorakiat, C., Paul, A., Sakdinawat, A. E., Murnane, M. M., Kapteyn, H. C., Miao, J., Schoenlein, R., Corkum, P., DeSilvestri, S., Nelson, K. A., Riedle, E. SPRINGER-VERLAG BERLIN. 2009: 146-+

    View details for Web of Science ID 000282108000048

  • Near diffraction limited coherent diffractive imaging with tabletop soft x-ray sources Sandberg, R. L., Raymondson, D. A., Schlotter, W. F., Raines, K., La-O-Vorakiat, C., Paul, A., Murnane, M. M., Kapteyn, H. C., Miao, J., David, C., Nolting, F., Quitmann, C., Stampanoni, M., Pfeiffer, F. IOP PUBLISHING LTD. 2009

    View details for DOI 10.1088/1742-6596/186/1/012058

    View details for Web of Science ID 000282023900058

  • Extended field of view soft x-ray Fourier transform holography: toward imaging ultrafast evolution in a single shot. Optics letters Schlotter, W. F., Lüning, J. n., Rick, R. n., Chen, K. n., Scherz, A. n., Eisebitt, S. n., Günther, C. M., Eberhardt, W. n., Hellwig, O. n., Stöhr, J. n. 2007; 32 (21): 3110–12

    Abstract

    Panoramic full-field imaging is demonstrated by applying spatial multiplexing to Fourier transform holography. Multiple object and reference waves extend the effective field of view for lensless imaging without compromising the spatial resolution. In this way, local regions of interest distributed throughout a sample can be simultaneously imaged with high spatial resolution. A method is proposed for capturing multiple ultrafast images of a sample with a single x-ray pulse.

    View details for PubMedID 17975613