Catalysis in real time using X-ray lasers

Nilsson, Anders; LaRue, Jerry; Öberg, Henrik; Ogasawara, Hirohito; Dell’Angela, Martina; Beye, Martin; Öström, Henrik; Gladh, Jörgen; Nørskov, Jens K.; Würth, W.; Abild‐Pedersen, Frank; Pettersson, Lars G. M.

doi:10.1016/j.cplett.2017.02.018

Cited by 49 publications

(32 citation statements)

References 93 publications

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“…In combination with the high chemical specificity and surface sensitivity of photoelectron spectroscopy and together with the femtosecond duration of XFEL pulses, these experiments open up the possibility of obtaining direct ultrafast structural information of reactants involved in chemical reactions at surfaces. Time-resolved structural data will enormously contribute to the fundamental understanding of more complex processes in heterogeneous catalysis both on single metal crystals [53] and more exotic layered crystals as perovskites [54], leading eventually to more efficient catalysts. In addition, time-resolved XSW may reveal the structural dynamics at the basis of light-induced superconductivity [55][56][57] by providing element and site specific atomic positions [58][59][60] as a function of the delay from the light pump pulse.…”

Section: Resultsmentioning

confidence: 99%

Surface structure determination by x-ray standing waves at a free-electron laser

et al. 2019

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We demonstrate the structural sensitivity and accuracy of the x-ray standing wave technique at a high repetition rate free-electron laser, FLASH at DESY in Hamburg, by measuring the photoelectron yield from the surface SiO 2 of Mo/Si multilayers. These experiments open up the possibility to obtain unprecedented structural information of adsorbate and surface atoms with picometer spatial and femtosecond temporal resolution. This technique will substantially contribute to a fundamental understanding of chemical reactions at catalytic surfaces and the structural dynamics of superconductors.

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Section: Resultsmentioning

confidence: 99%

Surface structure determination by x-ray standing waves at a free-electron laser

et al. 2019

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“…[89,90] These measurements represent the first structurally-sensitive experiments able to probe transition states in chemical reactions during catalytically-active processes. [91] A second class of experiments has investigated photochemical processes of species in solution using resonant inelastic X-ray scattering (RIXS) in the soft X-ray regime. This has allowed researchers to follow the most fundamental of chemical processes: bond-breaking and bond-making.…”

Section: Athosmentioning

confidence: 99%

Opportunities for Chemistry at the SwissFEL X-ray Free Electron Laser

Milne¹,

Beaud

Deng

et al. 2017

Chimia

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X-ray techniques have long been applied to chemical research, ranging from powder diffraction tools to analyse material structure to X-ray fluorescence measurements for sample composition. The development of high-brightness, accelerator-based X-ray sources has allowed chemists to use similar techniques but on more demanding samples and using more photon-hungry methods. X-ray Free Electron Lasers (XFELs) are the latest in the development of these large-scale user facilities, opening up new avenues of research and the possibility of more advanced applications for a range of research. The SwissFEL XFEL project at the Paul Scherrer Institute will begin user operation in the hard X-ray (2.1-12.4 keV) photon energy range in 2018 with soft X-ray (240-1930 eV) user operation to follow and here we will present the details of this project, it's operating capabilities, and some aspects of the experimental stations that will be particularly attractive for chemistry research. SwissFEL is a revolutionary new machine that will complement and extend the time-resolved chemistry efforts in the Swiss research community.

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“…Furthermore, we can envision X-ray pump X-ray spectroscopy probe experiments with few femtosecond time resolution to monitor the valence electronic structure of adsorbates after selective activation by soft X-rays. [28][29][30][31] In this work, we take a first step toward this vision and report on CO oxidation on Ru(0001) driven by resonant soft X-ray excitation. We use a single pulse as well as a sequence of two 30 fs delayed X-ray pulses (double pulse) of a few femtosecond duration at different intensities to drive CO oxidation.…”

Section: Introductionmentioning

confidence: 99%

Atom-specific activation in CO oxidation

Schreck

Diesen

LaRue

et al. 2018

The Journal of Chemical Physics

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We report on atom-specific activation of CO oxidation on Ru(0001) via resonant X-ray excitation. We show that resonant 1s core-level excitation of atomically adsorbed oxygen in the co-adsorbed phase of CO and oxygen directly drives CO oxidation. We separate this direct resonant channel from indirectly driven oxidation via X-ray induced substrate heating. Based on density functional theory calculations, we identify the valence-excited state created by the Auger decay as the driving electronic state for direct CO oxidation. We utilized the fresh-slice multi-pulse mode at the Linac Coherent Light Source that provided time-overlapped and 30 fs delayed pairs of soft X-ray pulses and discuss the prospects of femtosecond X-ray pump X-ray spectroscopy probe, as well as X-ray twopulse correlation measurements for fundamental investigations of chemical reactions via selective X-ray excitation.

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Catalysis in real time using X-ray lasers

Cited by 49 publications

References 93 publications

Surface structure determination by x-ray standing waves at a free-electron laser

Surface structure determination by x-ray standing waves at a free-electron laser

Opportunities for Chemistry at the SwissFEL X-ray Free Electron Laser

Atom-specific activation in CO oxidation

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