Time-Resolved Fluorescence and Absorption Spectroscopy of Photosystem I

Picosecond fluorescence and femtosecond transient absorption spectroscopy have been used to investigate the primary energy transfer and trapping processes in a photosystem II deletion mutant from the cyanobacterium Synechocystis sp. PCC 6803, which contains active photosystem I reaction centers with ∼ 100 chlorophylls per P700. In all experiments, low levels of excitation were used which avoid annihilation processes. Following 590-nm excitation, at room temperature, spectral equilibration is observed in both fluorescence and absorption measurements and is characterized by a time constant of 4–6 ps. The shape of the spectra associated with the equilibration process indicates that long wavelength pigments (pigments with absorption maxima at longer wavelength than that of the primary electron donor, P700) are present and functional at physiological temperatures in this preparation. The overall decay of excitations in the antenna is characterized by a time constant of 24–28 ps, in both fluorescence and absorption measurements. The 24–28-ps process results in the appearance of absorption changes associated with only P700⁺ formation. Absorption changes associated with the reduction of the primary electron acceptor were not resolved under the experimental conditions used here.