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

Kunnus, Kristjan; Josefsson, Ida; Rajkovic, Ivan; Schreck, Simon; Quevedo, Wilson; Beye, Martin; Grübel, Sebastian; Scholz, Mirko; Nordlund, Dennis and Zhang, Wenkai, et al. (2016) In New Journal of Physics 18(10).
Abstract

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... (More)

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.

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publication status
published
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keywords
anti-Stokes resonant x-ray raman scattering, excited state selectivity, free electron lasers, resonant inelastic x-ray scattering, ultrafast photochemistry
in
New Journal of Physics
volume
18
issue
10
publisher
IOP Publishing Ltd.
external identifiers
  • scopus:84992718295
ISSN
1367-2630
DOI
10.1088/1367-2630/18/10/103011
language
English
LU publication?
yes
id
621d04a0-1239-497a-8519-6f7bf588c438
date added to LUP
2016-11-16 14:08:31
date last changed
2017-10-01 05:25:57
@article{621d04a0-1239-497a-8519-6f7bf588c438,
  abstract     = {<p>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)<sub>5</sub> 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.</p>},
  articleno    = {103011},
  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},
  issn         = {1367-2630},
  keyword      = {anti-Stokes resonant x-ray raman scattering,excited state selectivity,free electron lasers,resonant inelastic x-ray scattering,ultrafast photochemistry},
  language     = {eng},
  month        = {10},
  number       = {10},
  publisher    = {IOP Publishing Ltd.},
  series       = {New Journal of Physics},
  title        = {Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics},
  url          = {http://dx.doi.org/10.1088/1367-2630/18/10/103011},
  volume       = {18},
  year         = {2016},
}