Primary Processes and Structure of the Photosystem II Reaction Center. 4. Low-Intensity Femtosecond Transient Absorption Spectra of D1-D2-cyt-b559 Reaction Centers†,‡

Low-intensity transient absorption spectroscopy has been performed on the isolated D1-D2-cyt-b559 reaction center complex of photosystem II from spinach. The excitation intensity was low enough to keep annihilation at a relatively low level (∼11%) and still maintain a very high signal/noise ratio. The kinetics has been measured with ∼200 fs resolution over two time ranges extending up to 200 ps for two different excitation wavelengths (680 nm, preferential primary donor excitation, and 670 nm, preferential external chlorophyll excitation). Detection wavelengths both in the pheophytin Qx region (535−555 nm) and in the chlorin Qy region, including the stimulated emission range (660−760 nm) have been employed. The data for all excitation/detection wavelength pairs and from both time ranges have been analyzed by combined global analysis. A highly complex kinetics, i.e. six lifetimes, has been found necessary for a good description of the data over the entire excitation/detection matrix and time range. These l...

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