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Title: Fingerprints of electronic, spin and structural dynamics from resonant inelastic soft X-ray scattering in transient photo-chemical species

Here, we describe how inversion symmetry separation of electronic state manifolds in resonant inelastic soft X-ray scattering (RIXS) can be applied to probe excited-state dynamics with compelling selectivity. In a case study of Fe L 3-edge RIXS in the ferricyanide complex Fe(CN) 6 3-, we demonstrate with multi-configurational restricted active space spectrum simulations how the information content of RIXS spectral fingerprints can be used to unambiguously separate species of different electronic configurations, spin multiplicities, and structures, with possible involvement in the decay dynamics of photo-excited ligand-to-metal charge-transfer. Specifically, we propose that this could be applied to confirm or reject the presence of a hitherto elusive transient Quartet species. Thus, RIXS offers a particular possibility to settle a recent controversy regarding the decay pathway, and we expect the technique to be similarly applicable in other model systems of photo-induced dynamics.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ;  [3] ; ORCiD logo [4] ;  [5] ;  [6] ; ORCiD logo [3] ; ORCiD logo [7] ;  [4] ; ORCiD logo [1]
  1. Stockholm Univ. (Sweden). Department of Physics, AlbaNova University Center
  2. Universität Potsdam, Institut für Physik und Astronomie (Germany)
  3. Institute for Methods and Instrumentation for Synchrotron Radiation Research, Berlin (Germany). Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
  4. Universität Potsdam, Institut für Physik und Astronomie (Germany); Institute for Methods and Instrumentation for Synchrotron Radiation Research, Berlin (Germany). Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
  5. Uppsala Univ. (Sweden). Department of Chemistry – Ångström Laboratory
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource; Stanford Univ., CA (United States). PULSE Institute
  7. Uppsala Univ. (Sweden). Department of Chemistry – Ångström Laboratory; Univ. of Siena (Italy). Department of Biotechnology, Chemistry and Pharmacy
Publication Date:
Grant/Contract Number:
AC02-76SF00515; 2015-03956; KAW- 2013.0020; VI 419; 669531
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 20; Journal Issue: 10; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1436985