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Wide-band TA maps an Fe(II) four-state cascade
Femtosecond TA from 370–1200 nm resolves 1PALCT → 3PALCT → 3MC → 5MC decay in an iron amido chromophore, including a ~100 fs NIR CT signature.
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What complex is the low-spin photosensitizer?
(CF3L1)2Fe, a pseudo-octahedral low-spin 3d6 Fe(II) amido chromophore.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
What does (CF3L2)2Fe model?
The high-spin 5MC ligand-field state of the photoexcited analogue.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
Pump and probe conditions?
600 nm pump, 370–1200 nm probe, ~0.3 mM in toluene.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
Where is PALCT ESA strongest?
A broad band ~800–1200 nm at early delays.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
PALCT → MC time constant?
About 100 fs from the NIR decay.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
What even faster step is assigned?
1PALCT → 3PALCT ISC (~50 fs), limited by the IRF.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
Evidence for 3MC → 5MC?
Isosbestic point at 545 nm between 175 and 325 fs (~250 fs component).
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
How long does 5MC live?
Major component ~3.5 ns before ground-state recovery.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
What oscillations are seen?
Impulsive Raman modes at 60, 80, and 110 cm–1 in the ground state.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
Why is this cascade like Fe(bpy)3?
Same 1CT → 3CT → 3MC → 5MC order established for d6 polypyridyls.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified
Visible λmax of the high-spin analogue?
470 nm with ε = 23 600 M–1 cm–1.
Source: Resolving consecutive excited-state evolution in Fe-amido chromophores by wide-band optical transient absorption spectroscopy · DOI · quote verified