TY  - JOUR
A1  - Sellberg, Jonas A.
A1  - McQueen, Trevor A.
A1  - Laksmono, Hartawan
A1  - Schreck, Simon
A1  - Beye, Martin
A1  - DePonte, Daniel P.
A1  - Kennedy, Brian
A1  - Nordlund, Dennis
A1  - Sierra, Raymond G.
A1  - Schlesinger, Daniel
A1  - Tokushima, Takashi
A1  - Zhovtobriukh, Iurii
A1  - Eckert, Sebastian
A1  - Segtnan, Vegard H.
A1  - Ogasawara, Hirohito
A1  - Kubicek, Katharina
A1  - Techert, Simone
A1  - Bergmann, Uwe
A1  - Dakovski, Georgi L.
A1  - Schlotter, William F.
A1  - Harada, Yoshihisa
A1  - Bogan, Michael J.
A1  - Wernet, Philippe
A1  - Föhlisch, Alexander
A1  - Pettersson, Lars G. M.
A1  - Nilsson, Anders
T1  - X-ray emission spectroscopy of bulk liquid water in "no-man's land"
JF  - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr
N2  - The structure of bulk liquid water was recently probed by x-ray scattering below the temperature limit of homogeneous nucleation (T-H) of similar to 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 T-H 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 1b(1)' and 1b(1)" 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. (C) 2015 AIP Publishing LLC.
Y1  - 2015
U6  - https://doi.org/10.1063/1.4905603
SN  - 0021-9606
SN  - 1089-7690
VL  - 142
IS  - 4
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Dell'Angela, Martina
A1  - Anniyev, Toyli
A1  - Beye, Martin
A1  - Coffee, Ryan
A1  - Föhlisch, Alexander
A1  - Gladh, Jörgen
A1  - Kaya, Sarp
A1  - Katayama, Tetsuo
A1  - Krupin, Oleg
A1  - Nilsson, Anders
A1  - Nordlund, Dennis
A1  - Schlotter, William F.
A1  - Sellberg, Jonas A.
A1  - Sorgenfrei, Florian
A1  - Turner, Joshua J.
A1  - ÖstrÖm, Henrik
A1  - Ogasawara, Hirohito
A1  - Wolf, Martin
A1  - Wurth, Wilfried
T1  - Vacuum space charge effects in sub-picosecond soft X-ray photoemission on a molecular adsorbate layer
JF  - Structural dynamics
N2  - Vacuum space charge induced kinetic energy shifts of O 1s and Ru 3d core levels in femtosecond soft X-ray photoemission spectra (PES) have been studied at a free electron laser (FEL) for an oxygen layer on Ru(0001). We fully reproduced the measurements by simulating the in-vacuum expansion of the photoelectrons and demonstrate the space charge contribution of the high-order harmonics in the FEL beam. Employing the same analysis for 400 nm pump-X-ray probe PES, we can disentangle the delay dependent Ru 3d energy shifts into effects induced by space charge and by lattice heating from the femtosecond pump pulse. (C) 2015 Author(s).
Y1  - 2015
U6  - https://doi.org/10.1063/1.4914892
SN  - 2329-7778
VL  - 2
IS  - 2
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Eckert, Sebastian
A1  - Norell, Jesper
A1  - Miedema, Piter S.
A1  - Beye, Martin
A1  - Fondell, Mattis
A1  - Quevedo, Wilson
A1  - Kennedy, Brian
A1  - Hantschmann, Markus
A1  - Pietzsch, Annette
A1  - van Kuiken, Benjamin
A1  - Ross, Matthew
A1  - Minitti, Michael P.
A1  - Moeller, Stefan P.
A1  - Schlotter, William F.
A1  - Khalil, Munira
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Untersuchung unabhängiger N‐H‐ und N‐C‐Bindungsverformungen auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung
JF  - Angewandte Chemie
N2  - Die Femtosekundendynamik nach resonanten Photoanregungen mit optischen und Röntgenpulsen ermöglicht eine selektive Verformung von chemischen N‐H‐ und N‐C‐Bindungen in 2‐Thiopyridon in wässriger Lösung. Die Untersuchung der orbitalspezifischen elektronischen Struktur und ihrer Dynamik auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung an der N1s‐Resonanz am Synchrotron und dem Freie‐Elektronen‐Laser LCLS in Kombination mit quantenchemischen Multikonfigurationsberechnungen erbringen den direkten Nachweis dieser kontrollierten photoinduzierten Molekülverformungen und ihrer ultrakurzen Zeitskala.
KW  - Photochemie
KW  - Protonierung
KW  - RIXS (resonante inelastische Röntgenstreuung)
KW  - Selektiver Bindungsbruch
KW  - Stickstoff
Y1  - 2017
U6  - https://doi.org/10.1002/ange.201700239
SN  - 1521-3757
SN  - 1521-3773
VL  - 129
IS  - 22
SP  - 6184
EP  - 6188
ER  - 
TY  - GEN
A1  - Eckert, Sebastian
A1  - Norell, Jesper
A1  - Miedema, Piter S.
A1  - Beye, Martin
A1  - Fondell, Mattis
A1  - Quevedo, Wilson
A1  - Kennedy, Brian
A1  - Hantschmann, Markus
A1  - Pietzsch, Annette
A1  - van Kuiken, Benjamin E.
A1  - Ross, Matthew
A1  - Minitti, Michael P.
A1  - Moeller, Stefan P.
A1  - Schlotter, William F.
A1  - Khalil, Munira
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Untersuchung unabhängiger N‐H‐ und N‐C‐Bindungsverformungen auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung
T2  - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe
N2  - Die Femtosekundendynamik nach resonanten Photoanregungen mit optischen und Röntgenpulsen ermöglicht eine selektive Verformung von chemischen N‐H‐ und N‐C‐Bindungen in 2‐Thiopyridon in wässriger Lösung. Die Untersuchung der orbitalspezifischen elektronischen Struktur und ihrer Dynamik auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung an der N1s‐Resonanz am Synchrotron und dem Freie‐Elektronen‐Laser LCLS in Kombination mit quantenchemischen Multikonfigurationsberechnungen erbringen den direkten Nachweis dieser kontrollierten photoinduzierten Molekülverformungen und ihrer ultrakurzen Zeitskala.
T3  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1121 
KW  - Photochemie
KW  - Protonierung
KW  - RIXS (resonante inelastische Röntgenstreuung)
KW  - Selektiver Bindungsbruch
KW  - Stickstoff
Y1  - 2021
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-436688
SN  - 1866-8372
IS  - 1121
ER  - 
TY  - JOUR
A1  - Eckert, Sebastian
A1  - Norell, Jesper
A1  - Miedema, Piter S.
A1  - Beye, Martin
A1  - Fondell, Mattis
A1  - Quevedo, Wilson
A1  - Kennedy, Brian
A1  - Hantschmann, Markus
A1  - Pietzsch, Annette
A1  - Van Kuiken, Benjamin E.
A1  - Ross, Matthew
A1  - Minitti, Michael P.
A1  - Moeller, Stefan P.
A1  - Schlotter, William F.
A1  - Khalil, Munira
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering
JF  - Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition
N2  - 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 time-scale.
KW  - nitrogen
KW  - photochemistry
KW  - protonation
KW  - RIXS (resonant inelastic X-ray scattering)
KW  - selective bond cleavage
Y1  - 2017
U6  - https://doi.org/10.1002/anie.201700239
SN  - 1433-7851
SN  - 1521-3773
VL  - 56
SP  - 6088
EP  - 6092
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - GEN
A1  - Eckert, Sebastian
A1  - Norell, Jesper
A1  - Miedema, Piter S.
A1  - Beye, Martin
A1  - Fondell, Mattis
A1  - Quevedo, Wilson
A1  - Kennedy, Brian
A1  - Hantschmann, Markus
A1  - Pietzsch, Annette
A1  - van Kuiken, Benjamin E.
A1  - Ross, Matthew
A1  - Minitti, Michael P.
A1  - Moeller, Stefan P.
A1  - Schlotter, William F.
A1  - Khalil, Munira
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Ultrafast Independent N-H and N-C Bond Deformation Investigated with Resonant Inelastic X-Ray Scattering
T2  - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe
N2  - 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 time-scale.
T3  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1115 
KW  - nitrogen
KW  - photochemistry
KW  - protonation
KW  - RIXS (resonant inelastic X-ray scattering)
KW  - selective bond cleavage
Y1  - 2021
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-436873
SN  - 1866-8372
IS  - 1115
ER  - 
TY  - JOUR
A1  - Xin, Hong
A1  - LaRue, Jerry
A1  - Oberg, Henrik
A1  - Beye, Martin
A1  - Turner, J. J.
A1  - Gladh, Jörgen
A1  - Ng, May L.
A1  - Sellberg, Jonas A.
A1  - Kaya, Sarp
A1  - Mercurio, G.
A1  - Hieke, F.
A1  - Nordlund, Dennis
A1  - Schlotter, William F.
A1  - Dakovski, Georgi L.
A1  - Minitti, Michael P.
A1  - Föhlisch, Alexander
A1  - Wolf, Martin
A1  - Wurth, Wilfried
A1  - Ogasawara, Hirohito
A1  - Norskov, Jens K.
A1  - Ostrom, Henrik
A1  - Pettersson, Lars G. M.
A1  - Nilsson, Anders
A1  - Abild-Pedersen, Frank
T1  - Strong Influence of Coadsorbate Interaction on CO Desorption Dynamics on Ru(0001) Probed by Ultrafast X-Ray Spectroscopy and Ab Initio Simulations
JF  - Physical review letters
N2  - We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distribution and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5 sigma and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process.
Y1  - 2015
U6  - https://doi.org/10.1103/PhysRevLett.114.156101
SN  - 0031-9007
SN  - 1079-7114
VL  - 114
IS  - 15
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Schreck, Simon
A1  - Beye, Martin
A1  - Sellberg, Jonas A.
A1  - McQueen, Trevor
A1  - Laksmono, Hartawan
A1  - Kennedy, Brian
A1  - Eckert, Sebastian
A1  - Schlesinger, Daniel
A1  - Nordlund, Dennis
A1  - Ogasawara, Hirohito
A1  - Sierra, Raymond G.
A1  - Segtnan, Vegard H.
A1  - Kubicek, Katharina
A1  - Schlotter, William F.
A1  - Dakovski, Georgi L.
A1  - Moeller, Stefan P.
A1  - Bergmann, Uwe
A1  - Techert, Simone
A1  - Pettersson, Lars G. M.
A1  - Wernet, Philippe
A1  - Bogan, Michael J.
A1  - Harada, Yoshihisa
A1  - Nilsson, Anders
A1  - Föhlisch, Alexander
T1  - Reabsorption of soft x-ray emission at high x-ray free-electron laserfluences
JF  - Physical review letters
N2  - 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.
Y1  - 2014
U6  - https://doi.org/10.1103/PhysRevLett.113.153002
SN  - 0031-9007
SN  - 1079-7114
VL  - 113
IS  - 15
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Eckert, Sebastian
A1  - Beye, Martin
A1  - Pietzsch, Annette
A1  - Quevedo, Wilson
A1  - Hantschmann, Markus
A1  - Ochmann, Miguel
A1  - Ross, Matthew
A1  - Minitti, Michael P.
A1  - Turner, Joshua J.
A1  - Moeller, Stefan P.
A1  - Schlotter, William F.
A1  - Dakovski, Georgi L.
A1  - Khalil, Munira
A1  - Huse, Nils
A1  - Föhlisch, Alexander
T1  - Principles of femtosecond X-ray/optical cross-correlation with X-ray induced transient optical reflectivity in solids
JF  - Applied physics letters
N2  - The discovery of ultrafast X-ray induced optical reflectivity changes enabled the development of X-ray/optical cross correlation techniques at X-ray free electron lasers worldwide. We have now linked through experiment and theory the fundamental excitation and relaxation steps with the transient optical properties in finite solid samples. Therefore, we gain a thorough interpretation and an optimized detection scheme of X-ray induced changes to the refractive index and the X-ray/optical cross correlation response. (C) 2015 AIP Publishing LLC.
Y1  - 2015
U6  - https://doi.org/10.1063/1.4907949
SN  - 0003-6951
SN  - 1077-3118
VL  - 106
IS  - 6
PB  - American Institute of Physics
CY  - Melville
ER  - 
TY  - JOUR
A1  - Wernet, Philippe
A1  - Kunnus, Kristjan
A1  - Josefsson, Ida
A1  - Rajkovic, Ivan
A1  - Quevedo, Wilson
A1  - Beye, Martin
A1  - Schreck, Simon
A1  - Gruebel, S.
A1  - Scholz, Mirko
A1  - Nordlund, Dennis
A1  - Zhang, Wenkai
A1  - Hartsock, Robert W.
A1  - Schlotter, William F.
A1  - Turner, Joshua J.
A1  - Kennedy, Brian
A1  - Hennies, Franz
A1  - de Groot, Frank M. F.
A1  - Gaffney, Kelly J.
A1  - Techert, Simone
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Orbital-specific mapping of the ligand exchange dynamics of Fe(CO)(5) in solution
JF  - Nature : the international weekly journal of science
N2  - Transition-metal complexes have long attracted interest for fundamental chemical reactivity studies and possible use in solar energy conversion(1,2). Electronic excitation, ligand loss from the metal centre, or a combination of both, creates changes in charge and spin density at the metal site(3-11) that need to be controlled to optimize complexes for photocatalytic hydrogen production(8) and selective carbon-hydrogen bond activation(9-11). An understanding at the molecular level of how transition-metal complexes catalyse reactions, and in particular of the role of the short-lived and reactive intermediate states involved, will be critical for such optimization. However, suitable methods for detailed characterization of electronic excited states have been lacking. Here we show, with the use of X-ray laser-based femtosecond-resolution spectroscopy and advanced quantum chemical theory to probe the reaction dynamics of the benchmark transition-metal complex Fe(CO)(5) in solution, that the photo-induced removal of CO generates the 16-electron Fe(CO)(4) species, a homogeneous catalyst(12,13) with an electron deficiency at the Fe centre(14,15), in a hitherto unreported excited singlet state that either converts to the triplet ground state or combines with a CO or solvent molecule to regenerate a penta-coordinated Fe species on a sub-picosecond timescale. This finding, which resolves the debate about the relative importance of different spin channels in the photochemistry of Fe(CO)(5) (refs 4, 16-20), was made possible by the ability of femtosecond X-ray spectroscopy to probe frontier-orbital interactions with atom specificity. We expect the method to be broadly applicable in the chemical sciences, and to complement approaches that probe structural dynamics in ultrafast processes.
Y1  - 2015
U6  - https://doi.org/10.1038/nature14296
SN  - 0028-0836
SN  - 1476-4687
VL  - 520
IS  - 7545
SP  - 78
EP  - 81
PB  - Nature Publ. Group
CY  - London
ER  -