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MO: Fachverband Molekülphysik

MO 21: Electronic Spectroscopy I

MO 21.3: Talk

Thursday, March 17, 2011, 11:00–11:15, MER 02

Sub-Femtosecond Electron Delocalization between Fe³⁺ and H₂O versus D₂O Solvents — •Tom Stalinski¹, Sébastien Bonhommeau², Samira Ghadimi¹, Kathrin Lange¹, Alexander Kothe¹, René Könnecke¹, Kai Hodeck¹, Majed Chergui³, and Emad Aziz^1,4 — ¹Helmholtz-Zentrum Berlin für Materialien und Energie, c/o BESSY GmbH, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany — ²Institut des Sciences Moléculaires, UMR 5255 CNRS, Université Bordeaux 1, 351 cours de la Libération, F-33405 Talence Cedex, France — ³Ecole Polytechnique Fédérale de Lausanne, Laboratoire de Spectroscopie Ultrarapide, Faculté des Sciences de Base, ISIC, Station 6, CH-1015 Lausanne, Switzerland — ⁴Freie Universität Berlin, FB Physik, Arnimallee 14, D-14195 Berlin, Germany

Charge transfer processes from aqueous Fe³⁺ ions to solvent molecules have been reported by using dark channel fluorescence-yield (DCFY) spectroscopy at the L-Edge. It was found that the interaction with the water solvent molecule around this ion leads to an appearance of a dip feature in the L₃-edge of the fluorescence yield[1]. Here we report on the difference between Fe³⁺ ions dissolved in water (H₂O) versus heavy water (D₂O) as revealed by fluorescence yield L-edge X-ray absorption spectroscopy of these two systems. Comparison with the corresponding transmission absorption spectra and Multiplet Calculations are used to quantify the DCFY mechanism. Furthermore core-hole lifetimes of the involved states are estimated in a sub-femtosecond timescale. [1]: E. F. Aziz et al.,Nature Chemistry 2, 853 (2010).