Identification of an additional low-lying excited state of carotenoid radical cations.

  • Prize N
  • Polívka T
  • Kaligotla S
 et al. 
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Abstract

Excited state dynamics of two apo-carotenals, retinal and 12'-apo-β-carotenal, were studied by femtosecond transient absorption spectroscopy. We make use of previous knowledge gathered from studies of various carbonyl carotenoids and suggest that to consistently explain the excited-state dynamics of retinal in polar solvents, it is necessary to include an intermolecular charge transfer (ICT) state in the excited state manifold. Coupling of the ICT state to the A(g)(-) state, which occurs in polar solvents, shortens lifetime of the lowest excited state of 12'-apo-β-carotenal from 180 ps in n-hexane to 7.1 ps in methanol. Comparison with a reference molecule lacking the conjugated carbonyl group, 12'-apo-β-carotene, demonstrates the importance of the carbonyl group; no polarity-induced lifetime change is observed and 12'-apo-β-carotene decays to the ground state in 220 ps regardless of solvent polarity. For retinal, we have confirmed the well-known three-state relaxation scheme in n-hexane. Population of the B(u)(+) state decays in

Author-supplied keywords

  • Carotenoids
  • Carotenoids: chemistry
  • Cations
  • Cations: chemistry
  • Chlorophyll
  • Chlorophyll: chemistry
  • Free Radicals
  • Free Radicals: chemistry
  • Hexanes
  • Hexanes: chemistry
  • Methanol
  • Methanol: chemistry
  • Models
  • Molecular
  • Molecular Conformation
  • Photochemistry
  • Retinaldehyde
  • Retinaldehyde: chemistry
  • Spectrophotometry
  • Time Factors
  • carotenoid
  • excited state kinetics
  • ict state
  • molecular orbital theory
  • polyene spectroscopy

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Authors

  • Nobel Prize

  • Tomáš Polívka

  • Shanti Kaligotla

  • Pavel Chábera

  • Harry A Frank

  • Andreas Dreuw

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