@article{JayVazdaCruzEckertetal.2020,
  author    = {Jay, Raphael M. and Vaz da Cruz, Vinicius and Eckert, Sebastian and Fondell, Mattis and Mitzner, Rolf and F{\"o}hlisch, Alexander},
  title     = {Probing solute-solvent interactions of transition metal complexes using L-edge absorption spectroscopy},
  series = {The journal of physical chemistry : B, Condensed matter, materials, surfaces, interfaces \& biophysical chemistry},
  volume    = {124},
  journal   = {The journal of physical chemistry : B, Condensed matter, materials, surfaces, interfaces \& biophysical chemistry},
  number    = {27},
  publisher = {American Chemical Society},
  address   = {Washington},
  issn      = {1520-6106},
  doi       = {10.1021/acs.jpcb.0c00638},
  pages     = {5636 -- 5645},
  year      = {2020},
  abstract  = {In order to tailor solution-phase chemical reactions involving transition metal complexes, it is critical to understand how their valence electronic charge distributions are affected by the solution environment. Here, solute-solvent interactions of a solvatochromic mixed-ligand iron complex were investigated using X-ray absorption spectroscopy at the transition metal L-2,L-3-edge. Due to the selectivity of the corresponding core excitations to the iron 3d orbitals, the method grants direct access to the valence electronic structure around the iron center and its response to interactions with the solvent environment. A linear increase of the total L-2,L-3-edge absorption cross section as a function of the solvent Lewis acidity is revealed. The effect is caused by relative changes in different metal-ligand-bonding channels, which preserve local charge densities while increasing the density of unoccupied states around the iron center. These conclusions are corroborated by a combination of molecular dynamics and spectrum simulations based on time-dependent density functional theory. The simulations reproduce the spectral trends observed in the X-ray but also optical absorption experiments. Our results underscore the importance of solute-solvent interactions when aiming for an accurate description of the valence electronic structure of solvated transition metal complexes and demonstrate how L-2,L-3-edge absorption spectroscopy can aid in understanding the impact of the solution environment on intramolecular covalency and the electronic charge distribution.},
  language  = {en}
}
@misc{FondellEckertJayetal.2017,
  author    = {Fondell, Mattis and Eckert, Sebastian and Jay, Raphael Martin and Weniger, Christian and Quevedo, Wilson and Niskanen, Johannes and Kennedy, Brian and Sorgenfrei, Nomi and Schick, Daniel and Giangrisostomi, Erika and Ovsyannikov, Ruslan and Adamczyk, Katrin and Huse, Nils and Wernet, Philippe and Mitzner, Rolf and F{\"o}hlisch, Alexander},
  title     = {Time-resolved soft X-ray absorption spectroscopy in transmission mode on liquids at MHz repetition rates},
  series = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe},
  journal   = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe},
  number    = {780},
  issn      = {1866-8372},
  doi       = {10.25932/publishup-43752},
  url       = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-437529},
  pages     = {12},
  year      = {2017},
  abstract  = {We present a setup combining a liquid flatjet sample delivery and a MHz laser system for time-resolved soft X-ray absorption measurements of liquid samples at the high brilliance undulator beamline UE52-SGM at Bessy II yielding unprecedented statistics in this spectral range. We demonstrate that the efficient detection of transient absorption changes in transmission mode enables the identification of photoexcited species in dilute samples. With iron(II)-trisbipyridine in aqueous solution as a benchmark system, we present absorption measurements at various edges in the soft X-ray regime. In combination with the wavelength tunability of the laser system, the set-up opens up opportunities to study the photochemistry of many systems at low concentrations, relevant to materials sciences, chemistry, and biology.},
  language  = {en}
}