Photosystem I particles from a eukaryotic organism, the green alga Chlamydomonas reinhardtii CC 2696, were studied by transient hole-burning spectroscopy at room temperature. Global analysis of the spectra recorded after excitation of chlorophyll a molecules in Photosystem I at selected wavelengths between 670 and 710 nm reveals excitation dynamics with subpicosecond, 2−3 ps, and 20−23 ps components. The subpicosecond and 2−3 ps components are ascribed to energy equilibration within the core antenna, whereas the 20−23 ps component is ascribed to energy trapping by the reaction center. Energy equilibration components describe both uphill and downhill energy transfer depending of the excitation wavelength. The initial transient absorbance bands after direct excitation of the red tail of the Q y transition band of chlorophyll a (at 700, 705, and 710 nm) are 25 nm wide and structured, revealing strongly coupled excited states among a group of molecules, most likely reaction center chlorophyll molecules. Excitation at shorter wavelengths (670, 680, and 695 nm) results in only 5−7 nm wide initial absorbance bands originating from photobleaching and stimulated emission of antenna chlorophyll molecules. The results are compared to the excitation dynamics of Photosystem I from the cyanobacterium Synechocystis sp. PCC 6803. The most significant difference is that the 2−3 ps phase describes internal excitation dynamics within higher-energy antenna chlorophyll molecules in the algal PS I system rather than between bulk and red chlorophylls, as observed in cyanobacterial PS I. No indications of core antenna red pigments absorbing above 700 nm were found in the preparation from Chlamydomonas. Independent of excitation wavelength, after at most a few picoseconds, all excitons are distributed over the same pool of chlorophyll molecules centered at ∼682 nm.

We report the observation of two conformational states of closed RCs from Rhodobacter sphaeroides characterized by different P(+)H(A)(-) --> PH(A) charge recombination lifetimes, one of which is of subnanosecond value (700 +/- 200 ps). These states are also characterized by different primary charge separation lifetimes. It is proposed that the distinct conformations are related to two protonation states either of reduced secondary electron acceptor, Q(A)(-), or of a titratable amino acid residue localized near Q(A). The reaction centers in the protonated state are characterized by faster charge separation and slower charge recombination when compared to those in the unprotonated state. Both effects are explained in terms of the model assuming modulation of the free energy level of the state P(+)H(A)(-) by the charges on or near Q(A) and decay of the P(+)H(A)(-) state via the thermally activated P(+)B(A)(-) state.

We measured picosecond time-resolved fluorescence of intact Photosystem I complexes from Chlamydomonas reinhardtii and Arabidopsis thaliana. The antenna system of C. reinhardtii contains about 30-60 chlorophylls more than that of A. thaliana, but lacks the so-called red chlorophylls, chlorophylls that absorb at longer wavelength than the primary electron donor. In C. reinhardtii, the main lifetimes of excitation trapping are about 27 and 68 ps. The overall lifetime of C. reinhardtii is considerably shorter than in A. thaliana. We conclude that the amount and energies of the red chlorophylls have a larger effect on excitation trapping time in Photosystem I than the antenna size.