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

Conference · Fri Aug 01 04:00:00 EDT 2008

OSTI ID:1006395

Huse, N; Kim, T -K; Khalil, M; Jamula, L; McCusker, J K; Schoenlein, R W

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.

• Research Organization: Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, CA (US)
• Sponsoring Organization: Chemical Sciences Division
• DOE Contract Number: AC02-05CH11231
• OSTI ID: 1006395
• Report Number(s): LBNL-4264E
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ABSORPTION
CHEMISTRY
DOORS
PROBES
SPECTROSCOPY
SPIN
TRANSIENTS
X-RAY SOURCES
X-RAY SPECTROSCOPY
femtosecond
spin cross over
transition-metal
ultrafast
organo-metallic