Kinetically distinct three red chlorophylls in photosystem i of thermosynechococcus elongatus revealed by femtosecond time-resolved fluorescence spectroscopy at 15 K

Yutaka Shibata, Atsushi Yamagishi, Shunsuke Kawamoto, Tomoyasu Noji, Shigeru Itoh

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21 Citations (Scopus)

Abstract

Time-resolved fluorescence spectra of photosystem I (PS-I) trimeric complex isolated from a thermophilic cyanobacterium, Thermosynechococcus (T.) elongatus, were observed at 15 K over the time range from 100 fs to a few nanoseconds under P700-oxidized condition and 10 ps to a few nanoseconds under P700-reduced condition. Global-fitting analysis of the data of P700-oxidized condition revealed the existence of three kinetically different red chlorophylls (ChIs) having the energy-transfer times to P700+ of 6.1 ps (C 6.1 ps), 140 ps (C140 ps), and 360 ps (C 360 ps)- According to the spectral shape of DAS, C6.1 ps, C140 ps, and C360 ps were assigned to the previously reported red Chls with the absorption maxima at 715 nm (C715), 710 nm (C710), and 719 nm (C719), respectively. In PS-I containing P700+, ca. 60 Chls funnel the excitation energy into C6.1 ps in a subpicosecond time region at 15 K. The analysis of the present data together with the conclusions of the previous reports revealed that in PS-I containing a neutral P700 the direct energy transfer from the bulk Chls to P700 seems to dominate the energy-flow process. Simulation of the energy-transfer time to P700+ based on Förster theory suggested the dimeric Chls A32-B7 and A33-A34 as the most probable candidates for C140 ps (C710) and C 360 ps (C719), respectively. C6.1 ps (C715) was tentatively assigned to the dimeric Chl B24-B25 or A26-A27, for which the fastest energy transfer to P700+ was predicted from the simulation. However, the estimated energy-transfer times to P700+ for these dimeric Chls were 44-46 ps, which were still much slower than the observed value of 6.1 ps. A theoretical framework beyond the standard Förster theory might be required in order to account for the severe deviation.

Original languageEnglish
Pages (from-to)2954-2963
Number of pages10
JournalJournal of Physical Chemistry B
Volume114
Issue number8
DOIs
Publication statusPublished - 2010 Mar 4
Externally publishedYes

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

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