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Title: Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

Here, 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-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [7] ;  [8] ;  [9] ;  [10] ;  [9] ;  [9] ;  [9] ;  [9] ;  [5] ;  [11] ;  [12] ;  [5] ;  [2] ;  [13]
  1. Helmholtz-Zentrum Berlin GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. Stockholm Univ., Stockholm (Sweden)
  3. Max Planck Institute for Biophysical Chemistry, Gottingen (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Helmholtz-Zentrum Berlin GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany); Stockholm Univ. (Sweden)
  5. Helmholtz-Zentrum Berlin GmbH, Berlin (Germany)
  6. Helmholtz-Zentrum Berlin GmbH, Berlin (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  7. Max Planck Institute for Biophysical Chemistry, Gottingen (Germany); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  8. Max Planck Institute for Biophysical Chemistry, Gottingen (Germany); Univ. Siegen, Siegen (Germany)
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  10. SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Pennsylvania, Philadelphia, PA (United States)
  11. MAX-Lab, Lund (Sweden)
  12. Max Planck Institute for Biophysical Chemistry, Gottingen (Germany); Gottingen Univ., Gottingen (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  13. Helmholtz-Zentrum Berlin GmbH, Berlin (Germany); Univ. Potsdam, Potsdam (Germany)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; SFB1073-DFG; SFB755-DFG
Type:
Accepted Manuscript
Journal Name:
New Journal of Physics
Additional Journal Information:
Journal Volume: 18; Journal Issue: 10; Journal ID: ISSN 1367-2630
Publisher:
IOP Publishing
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; ultrafast photochemistry; excited state selectivity; anti-Stokes resonant x-ray raman scattering; free electron lasers; resonant inelastic x-ray scattering
OSTI Identifier:
1348238

Kunnus, Kristjan, Josefsson, Ida, Rajkovic, Ivan, Schreck, Simon, Quevedo, Wilson, Beye, Martin, Grübel, Sebastian, Scholz, Mirko, Nordlund, Dennis, Zhang, Wenkai, Hartsock, Robert W., Gaffney, Kelly J., Schlotter, William F., Turner, Joshua J., Kennedy, Brian, Hennies, Franz, Techert, Simone, Wernet, Philippe, Odelius, Michael, and Föhlisch, Alexander. Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics. United States: N. p., Web. doi:10.1088/1367-2630/18/10/103011.
Kunnus, Kristjan, Josefsson, Ida, Rajkovic, Ivan, Schreck, Simon, Quevedo, Wilson, Beye, Martin, Grübel, Sebastian, Scholz, Mirko, Nordlund, Dennis, Zhang, Wenkai, Hartsock, Robert W., Gaffney, Kelly J., Schlotter, William F., Turner, Joshua J., Kennedy, Brian, Hennies, Franz, Techert, Simone, Wernet, Philippe, Odelius, Michael, & Föhlisch, Alexander. Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics. United States. doi:10.1088/1367-2630/18/10/103011.
Kunnus, Kristjan, Josefsson, Ida, Rajkovic, Ivan, Schreck, Simon, Quevedo, Wilson, Beye, Martin, Grübel, Sebastian, Scholz, Mirko, Nordlund, Dennis, Zhang, Wenkai, Hartsock, Robert W., Gaffney, Kelly J., Schlotter, William F., Turner, Joshua J., Kennedy, Brian, Hennies, Franz, Techert, Simone, Wernet, Philippe, Odelius, Michael, and Föhlisch, Alexander. 2016. "Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics". United States. doi:10.1088/1367-2630/18/10/103011. https://www.osti.gov/servlets/purl/1348238.
@article{osti_1348238,
title = {Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics},
author = {Kunnus, Kristjan and Josefsson, Ida and Rajkovic, Ivan and Schreck, Simon and Quevedo, Wilson and Beye, Martin and Grübel, Sebastian and Scholz, Mirko and Nordlund, Dennis and Zhang, Wenkai and Hartsock, Robert W. and Gaffney, Kelly J. and Schlotter, William F. and Turner, Joshua J. and Kennedy, Brian and Hennies, Franz and Techert, Simone and Wernet, Philippe and Odelius, Michael and Föhlisch, Alexander},
abstractNote = {Here, 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-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.},
doi = {10.1088/1367-2630/18/10/103011},
journal = {New Journal of Physics},
number = 10,
volume = 18,
place = {United States},
year = {2016},
month = {10}
}