Unveiling the excited state energy transfer pathways in peridinin-chlorophyll a-protein by ultrafast multi-pulse transient absorption spectroscopy

Kipras Redeckas*, Vladislava Voiciuk, Donatas Zigmantas, Roger G. Hiller, Mikas Vengris

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

15 Citations (Scopus)

Abstract

Time-resolved multi-pulse methods were applied to investigate the excited state dynamics, the interstate couplings, and the excited state energy transfer pathways between the light-harvesting pigments in peridinin-chlorophyll a-protein (PCP). The utilized pump-dump-probe techniques are based on perturbation of the regular PCP energy transfer pathway. The PCP complexes were initially excited with an ultrashort pulse, resonant to the S0 → S2 transition of the carotenoid peridinin. A portion of the peridinin-based emissive intramolecular charge transfer (ICT) state was then depopulated by applying an ultrashort NIR pulse that perturbed the interaction between S1 and ICT states and the energy flow from the carotenoids to the chlorophylls. The presented data indicate that the peridinin S1 and ICT states are spectrally distinct and coexist in an excited state equilibrium in the PCP complex. Moreover, numeric analysis of the experimental data asserts ICT → Chl-a as the main energy transfer pathway in the photoexcited PCP systems.

Original languageEnglish
Pages (from-to)297-307
Number of pages11
JournalBiochimica et Biophysica Acta - Bioenergetics
Volume1858
Issue number4
DOIs
Publication statusPublished - 1 Apr 2017

Keywords

  • Peridinin-chlorophyll α-protein
  • Pump-probe
  • Pump-dump-probe
  • Intramolecular charge transfer
  • Excited state equilibrium
  • Excitation energy transfer

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