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* Faculty of Sciences, Division of Physics and Astronomy, Department of Biophysics, Vrije Universiteit, 1081 HV Amsterdam, The Netherlands;
Department of Physics, Adam Mickiewicz University, 61-614 Pozna
, Poland;
Istituto di Biofisica, CNR, Trento, c/o ITC Povo, Trento 38100, Italy;
Dipartimento Scientifico e Tecnologico, Università di Verona, 15-37134 Verona, Italy; and ¶ Université Aix-Marseille II, LGBP, Faculté des Sciences de Luminy, Département de Biologie, Case 901, 13288 Marseille, France
Correspondence: Address reprint requests to Rienk van Grondelle, Tel.: 31-20-444-7930; E-mail: rienk{at}nat.vu.nl.
EET in reconstituted Lhca4, a peripheral light-harvesting complex from Photosystem I of Arabidopsis thaliana, containing 10 chlorophylls and 2 carotenoids, was studied at room temperature by femtosecond transient absorption spectroscopy. Two spectral forms of Lut were observed in the sites L1 and L2, characterized by significantly different interactions with nearby chlorophyll a molecules. A favorable interpretation of these differences is that the efficiency of EET to Chls is about two times lower from the "blue" Lut in the site L1 than from the "red" Lut in the site L2 due to fast IC in the former case. A major part of the energy absorbed by the "red" Lut,
60%70%, is transferred to Chls on a sub-100-fs timescale from the state S2 but, in addition, minor EET from the hot S1 state within 400500 fs is also observed. EET from the S1 state to chlorophylls occurs also within 23 ps and is ascribed to Vio and/or "blue" Lut. EET from Chl b to Chl a is biphasic and characterized by time constants of
300 fs and 3.0 ps. These rates are ascribed to EET from Chl b spectral forms absorbing at
644 nm and
650 nm, respectively. About 25% of the excited Chls a decays very fastwithin
15 ps. This decay is proposed to be related to the presence of the interacting Chls A5 and B5 located next to the carotenoid in the site L2 and may imply some photoprotective role for Lhca4 in the photosystem I super-complex.
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