Journal
CHEMPHYSCHEM
Volume 18, Issue 5, Pages 465-469Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201601396
Keywords
ab initio calculations; photocatalysis; photoelectron spectroscopy; spin crossover; ultrafast non-adiabatic dynamics
Funding
- European Research Council [279344]
- Helmholtz-Gemeinschaft Grant [VH-NG-635]
- Deanship of Scientific Research, King Abdulaziz University [D-003-435]
- Deutsche Forschungsgemeinschaft [KU 952/10-1]
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Photoinduced spin-flip in Fe-II complexes is an ultrafast phenomenon that has the potential to become an alternative to conventional processing and magnetic storage of information. Following the initial excitation by visible light into the singlet metal-to-ligand charge-transfer state, the electronic transition to the high-spin quintet state may undergo different pathways. Here we apply ultrafast XUV (extreme ultraviolet) photoemission spectroscopy to track the low-to-high spin dynamics in the aqueous iron tris-bipyridine complex, [Fe(bpy)(3)](2+), by monitoring the transient electron density distribution among excited states with femtosecond time resolution. Aided by first-principles calculations, this approach enables us to reveal unambiguously both the sequential and direct de-excitation pathways from singlet to quintet state, with a branching ratio of 4.5:1.
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