Probing reaction dynamics of transition-metal complexes in solution via time-resolved soft x-ray spectroscopy

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We report the first time-resolved soft x-ray measurements of solvated transition-metal complexes. L-edge spectroscopy directly probes dynamic changes in ligand-field splitting of 3d orbitals associated with the spin transition, and mediated by changes in ligand-bonding. We report the first time-resolved soft x-ray spectroscopy of solution-phase molecular dynamics. Changes in ligand-field splitting and spin-state populations in 3d orbitals of the Fe{sup II} complex are directly probed via transient absorption changes of the Fe L{sub 2} and L{sub 3} edges following photo-induced metal-to-ligand charge transfer. With the emergence of high-flux ultrafast soft x-ray sources, details on interplay between atomic structure, electronic states, ... continued below

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Huse, N.; Kim, T.-K.; Khalil, M.; Jamula, L.; McCusker, J.K. & Schoenlein, R.W. August 1, 2008.

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We report the first time-resolved soft x-ray measurements of solvated transition-metal complexes. L-edge spectroscopy directly probes dynamic changes in ligand-field splitting of 3d orbitals associated with the spin transition, and mediated by changes in ligand-bonding. We report the first time-resolved soft x-ray spectroscopy of solution-phase molecular dynamics. Changes in ligand-field splitting and spin-state populations in 3d orbitals of the Fe{sup II} complex are directly probed via transient absorption changes of the Fe L{sub 2} and L{sub 3} edges following photo-induced metal-to-ligand charge transfer. With the emergence of high-flux ultrafast soft x-ray sources, details on interplay between atomic structure, electronic states, and spin contributions will be revealed. Our experimental approach opens the door to femtosecond soft x-ray investigations of liquid phase chemistry that have previously been inaccessible.

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  • 16th International Conference on Ultrafast Phenomena

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  • Report No.: LBNL-4264E
  • Grant Number: DE-AC02-05CH11231
  • Office of Scientific & Technical Information Report Number: 1006395
  • Archival Resource Key: ark:/67531/metadc838040

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  • August 1, 2008

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  • May 19, 2016, 3:16 p.m.

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  • July 26, 2016, 5:54 p.m.

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Huse, N.; Kim, T.-K.; Khalil, M.; Jamula, L.; McCusker, J.K. & Schoenlein, R.W. Probing reaction dynamics of transition-metal complexes in solution via time-resolved soft x-ray spectroscopy, article, August 1, 2008; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc838040/: accessed July 22, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.