Kristjan Kunnus, Ida Josefsson, Ivan Rajkovic, Simon Schreck, Wilson Quevedo, Martin Beye, Sebastian Grübel, Mirko Scholz, Dennis Nordlund, Wenkai Zhang, Robert W. Hartsock, Kelly J. Gaffney, William F. Schlotter, Joshua J. Turner, Brian Kennedy, Franz Hennies, Simone Techert, Philippe Wernet, Michael Odelius, Alexander Föhlisch
- Ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbital and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)(5) in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-rayUltrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbital and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO)(5) in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given-which will be covered experimentally by upcoming transform-limited x-ray sources.…
MetadatenAuthor details: | Kristjan KunnusORCiD, Ida Josefsson, Ivan Rajkovic, Simon Schreck, Wilson Quevedo, Martin BeyeORCiDGND, Sebastian Grübel, Mirko Scholz, Dennis Nordlund, Wenkai Zhang, Robert W. Hartsock, Kelly J. Gaffney, William F. Schlotter, Joshua J. Turner, Brian Kennedy, Franz Hennies, Simone Techert, Philippe Wernet, Michael OdeliusORCiD, Alexander FöhlischORCiDGND |
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DOI: | https://doi.org/10.1088/1367-2630/18/10/103011 |
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ISSN: | 1367-2630 |
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Title of parent work (English): | NEW JOURNAL OF PHYSICS |
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Publisher: | IOP Publ. Ltd. |
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Place of publishing: | Bristol |
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Publication type: | Article |
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Language: | English |
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Year of first publication: | 2016 |
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Publication year: | 2016 |
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Release date: | 2020/03/22 |
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Tag: | anti-Stokes resonant x-ray raman scattering; excited state selectivity; free electron lasers; resonant inelastic x-ray scattering; ultrafast photochemistry |
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Volume: | 18 |
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Number of pages: | 9 |
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Funding institution: | US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]; LCLS; Stanford University through the Stanford Institute for Materials Energy Sciences (SIMES); Lawrence Berkeley National Laboratory (LBNL); University of Hamburg through the BMBF priority program [FSP 301]; Center for Free Electron Laser Science (CFEL); Swedish Research Council; Carl Tryggers Foundation; Magnus Bergvall Foundation; ERC-ADG-Advanced Investigator EDAX under the Horizon EU Framework Programme for Research and Innovation [669531]; Volkswagen Stiftung; AMOS program within the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy; [SFB755-DFG]; [SFB1073-DFG] |
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Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
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Peer review: | Referiert |
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