Speaker
Dr
Ph Wernet
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Description
We present our recent results on how we follow both the occupied and unoccupied valence orbitals of dissociating Fe(CO)5 molecules in solution with femtosecond RIXS at the free electron laser LCLS (Stanford, USA).
A pump-laser wavelength of 267 nm is used for resonant metal-to-ligand charge transfer excitation. The evolution of the valence electronic structure is probed with RIXS at the Fe L-edge as Fe(CO)5 dissociates into Fe(CO)4 and CO in ethanol solution. We use a recently built set up with a liquid jet in vacuum and a soft x-ray RIXS spectrometer. Our results reveal the coupling of orbital population, chare transfer and structural dynamics during dissociation and solvation of the photoproducts up to 3 picoseconds after initiating the reaction. They give unique insight into the coordinatively unsaturated carbonyl intermediate Fe(CO)4 and give complete access to the dissociation dynamics of a fundamentally important chemical bond with sigma-donation and pi-back donation between the metal center and the carbonyl groups. We believe that femtosecond RIXS gives unique access to the coupling of transient electronic structure and nuclear dynamics during chemical reactions.
This contribution will conclude with recent and complementary results with steady-state RIXS on liquids and solutions obtained with the same experimental set up at BESSY II.
Please specify the session
RIXS
Please specify poster or talk
Talk
Primary author
Dr
Ph Wernet
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Co-authors
Dr
A Föhlisch
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Dr
B Kennedy
(MAX-lab, Lund University, 221 00 Lund, Sweden)
Dr
B Schlotter
(Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA)
Dr
C Weniger
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Dr
D Nordlund
(Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA)
Dr
E Suljoti
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Dr
F Hennies
(MAX-lab, Lund University, 221 00 Lund, Sweden)
Dr
F de Groot
(Inorganic Chemistry and Catalysis, Debye Institute of Nanomaterials Science, Department of Chemistry, Utrecht University, Sorbonnelaan 16, 3584 CA Utrecht, Netherlands)
Dr
I Josefsson
(FYSIKUM, Stockholm University, AlbaNova, S-106 91 Stockholm, Sweden)
Dr
I Rajkovic
(Max-Planck-Institute for Biophysical Chemistry, Am Fassberg 11 37077 Göttingen, Germany)
Dr
J Turner
(Linac Coherent Light Source, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA)
Dr
K Gaffney
(PULSE, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA)
Dr
K Kunnus
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Dr
M Beye
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Dr
M Odelius
(FYSIKUM, Stockholm University, AlbaNova, S-106 91 Stockholm, Sweden)
Dr
M Scholz
(Max-Planck-Institute for Biophysical Chemistry, Am Fassberg 11 37077 Göttingen, Germany)
Dr
R Hartsock
(PULSE, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA)
Dr
S Grübel
(Max-Planck-Institute for Biophysical Chemistry, Am Fassberg 11 37077 Göttingen, Germany)
Dr
S Schreck
(Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Albert-Einstein-Str. 15, 12489 Berlin, Germany)
Dr
S Techert
(Max-Planck-Institute for Biophysical Chemistry, Am Fassberg 11 37077 Göttingen, Germany)
Dr
W Quevedo
(Max-Planck-Institute for Biophysical Chemistry, Am Fassberg 11 37077 Göttingen, Germany)
Dr
W Zhang
(PULSE, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA)
