TY - JOUR A1 - de Jong, S. A1 - Kukreja, R. A1 - Trabant, C. A1 - Pontius, N. A1 - Chang, C. F. A1 - Kachel, T. A1 - Beye, Martin A1 - Sorgenfrei, Florian A1 - Back, C. H. A1 - Braeuer, B. A1 - Schlotter, W. F. A1 - Turner, J. J. A1 - Krupin, O. A1 - Doehler, M. A1 - Zhu, D. A1 - Hossain, M. A. A1 - Scherz, A. O. A1 - Fausti, D. A1 - Novelli, F. A1 - Esposito, M. A1 - Lee, W. S. A1 - Chuang, Y. D. A1 - Lu, D. H. A1 - Moore, R. G. A1 - Yi, M. A1 - Trigo, M. A1 - Kirchmann, P. A1 - Pathey, L. A1 - Golden, M. S. A1 - Buchholz, Marcel A1 - Metcalf, P. A1 - Parmigiani, F. A1 - Wurth, W. A1 - Föhlisch, Alexander A1 - Schuessler-Langeheine, Christian A1 - Duerr, H. A. T1 - Speed limit of the insulator-metal transition in magnetite JF - Nature materials N2 - As the oldest known magnetic material, magnetite (Fe3O4) has fascinated mankind for millennia. As the first oxide in which a relationship between electrical conductivity and fluctuating/localized electronic order was shown(1), magnetite represents a model system for understanding correlated oxides in general. Nevertheless, the exact mechanism of the insulator-metal, or Verwey, transition has long remained inaccessible(2-8). Recently, three- Fe- site lattice distortions called trimeronswere identified as the characteristic building blocks of the low-temperature insulating electronically ordered phase(9). Here we investigate the Verwey transition with pump- probe X- ray diffraction and optical reflectivity techniques, and show how trimerons become mobile across the insulator-metal transition. We find this to be a two- step process. After an initial 300 fs destruction of individual trimerons, phase separation occurs on a 1.5 +/- 0.2 ps timescale to yield residual insulating and metallic regions. This work establishes the speed limit for switching in future oxide electronics(10). Y1 - 2013 U6 - https://doi.org/10.1038/NMAT3718 SN - 1476-1122 SN - 1476-4660 VL - 12 IS - 10 SP - 882 EP - 886 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Dell'Angela, M. A1 - Anniyev, Toyli A1 - Beye, Martin A1 - Coffee, Ryan A1 - Föhlisch, Alexander A1 - Gladh, J. A1 - Katayama, T. A1 - Kaya, S. A1 - Krupin, O. A1 - LaRue, J. A1 - Mogelhoj, A. A1 - Nordlund, D. A1 - Norskov, J. K. A1 - Oberg, H. A1 - Ogasawara, H. A1 - Ostrom, H. A1 - Pettersson, Lars G. M. A1 - Schlotter, W. F. A1 - Sellberg, J. A. A1 - Sorgenfrei, Florian A1 - Turner, J. J. A1 - Wolf, M. A1 - Wurth, W. A1 - Nilsson, A. T1 - Real-time observation of surface bond breaking with an X-ray Laser JF - Science N2 - We used the Linac Coherent Light Source free-electron x-ray laser to probe the electronic structure of CO molecules as their chemisorption state on Ru(0001) changes upon exciting the substrate by using a femtosecond optical laser pulse. We observed electronic structure changes that are consistent with a weakening of the CO interaction with the substrate but without notable desorption. A large fraction of the molecules (30%) was trapped in a transient precursor state that would precede desorption. We calculated the free energy of the molecule as a function of the desorption reaction coordinate using density functional theory, including van der Waals interactions. Two distinct adsorption wells-chemisorbed and precursor state separated by an entropy barrier-explain the anomalously high prefactors often observed in desorption of molecules from metals. Y1 - 2013 U6 - https://doi.org/10.1126/science.1231711 SN - 0036-8075 VL - 339 IS - 6125 SP - 1302 EP - 1305 PB - American Assoc. for the Advancement of Science CY - Washington ER - TY - JOUR A1 - Katayama, T. A1 - Anniyev, Toyli A1 - Beye, Martin A1 - Coffee, Ryan A1 - Dell'Angela, M. A1 - Föhlisch, Alexander A1 - Gladh, J. A1 - Kaya, S. A1 - Krupin, O. A1 - Nilsson, A. A1 - Nordlund, D. A1 - Schlotter, W. F. A1 - Sellberg, J. A. A1 - Sorgenfrei, Florian A1 - Turner, J. J. A1 - Wurth, W. A1 - Öström, H. A1 - Ogasawara, H. T1 - Ultrafast soft X-ray emission spectroscopy of surface adsorbates using an X-ray free electron laser JF - Journal of electron spectroscopy and related phenomena : the international journal on theoretical and experimental aspects of electron spectroscopy N2 - We report on an experimental system designed to probe chemical reactions on solid surfaces on a sub-picosecond timescale using soft X-ray emission spectroscopy at the Linac Coherent Light Source (LCLS) free electron laser (FEL) at the SLAC National Accelerator Laboratory. We analyzed the O 1s X-ray emission spectra recorded from atomic oxygen adsorbed on a Ru(0001) surface at a synchrotron beamline (SSRL, BL13-2) and an FEL beamline (LCLS, SXR). We have demonstrated conditions that provide negligible amount of FEL induced damage of the sample. In addition we show that the setup is capable of tracking the temporal evolution of electronic structure during a surface reaction of submonolayer quantities of CO molecules desorbing from the surface. KW - X-ray emission spectroscopy KW - Surface science KW - Free electron laser KW - Ultrafast Y1 - 2013 U6 - https://doi.org/10.1016/j.elspec.2013.03.006 SN - 0368-2048 VL - 187 IS - 1 SP - 9 EP - 14 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Ostrom, H. A1 - Oberg, H. A1 - Xin, H. A1 - Larue, J. A1 - Beye, Martin A1 - Gladh, J. A1 - Ng, M. L. A1 - Sellberg, J. A. A1 - Kaya, S. A1 - Mercurio, G. A1 - Nordlund, D. A1 - Hantschmann, Markus A1 - Hieke, F. A1 - Kuehn, D. A1 - Schlotter, W. F. A1 - Dakovski, G. L. A1 - Turner, J. J. A1 - Minitti, M. P. A1 - Mitra, A. A1 - Moeller, S. P. A1 - Föhlisch, Alexander A1 - Wolf, M. A1 - Wurth, W. A1 - Persson, Mats A1 - Norskov, J. K. A1 - Abild-Pedersen, Frank A1 - Ogasawara, Hirohito A1 - Pettersson, Lars G. M. A1 - Nilsson, A. T1 - Probing the transition state region in catalytic CO oxidation on Ru JF - Science N2 - Femtosecond x-ray laser pulses are used to probe the carbon monoxide (CO) oxidation reaction on ruthenium (Ru) initiated by an optical laser pulse. On a time scale of a few hundred femtoseconds, the optical laser pulse excites motions of CO and oxygen (O) on the surface, allowing the reactants to collide, and, with a transient close to a picosecond (ps), new electronic states appear in the OK-edge x-ray absorption spectrum. Density functional theory calculations indicate that these result from changes in the adsorption site and bond formation between CO and O with a distribution of OC-O bond lengths close to the transition state (TS). After 1 ps, 10% of the CO populate the TS region, which is consistent with predictions based on a quantum oscillator model. Y1 - 2015 U6 - https://doi.org/10.1126/science.1261747 SN - 0036-8075 SN - 1095-9203 VL - 347 IS - 6225 SP - 978 EP - 982 PB - American Assoc. for the Advancement of Science CY - Washington ER - TY - JOUR A1 - Pontius, N. A1 - Kachel, T. A1 - Schüssler-Langeheine, C. A1 - Schlotter, W. F. A1 - Beye, Martin A1 - Sorgenfrei, Florian A1 - Chang, C. F. A1 - Föhlisch, Alexander A1 - Wurth, W. A1 - Metcalf, P. A1 - Leonov, I. A1 - Yaresko, A. A1 - Stojanovic, N. A1 - Berglund, Martin A1 - Guerassimova, N. A1 - Duesterer, S. A1 - Redlin, H. A1 - Duerr, H. A. T1 - Time-resolved resonant soft x-ray diffraction with free-electron lasers femtosecond dynamics across the Verwey transition in magnetite JF - Applied physics letters N2 - Resonant soft x-ray diffraction (RSXD) with femtosecond (fs) time resolution is a powerful tool for disentangling the interplay between different degrees of freedom in strongly correlated electron materials. It allows addressing the coupling of particular degrees of freedom upon an external selective perturbation, e. g., by an optical or infrared laser pulse. Here, we report a time-resolved RSXD experiment from the prototypical correlated electron material magnetite using soft x-ray pulses from the free-electron laser FLASH in Hamburg. We observe ultrafast melting of the charge-orbital order leading to the formation of a transient phase, which has not been observed in equilibrium. Y1 - 2011 U6 - https://doi.org/10.1063/1.3584855 SN - 0003-6951 VL - 98 IS - 18 PB - American Institute of Physics CY - Melville ER -