Femtosecond Spectroscopy of Chlorosome Antennas from the Green Photosynthetic Bacterium Chloroflexus aurantiacus

The antenna kinetics of bacteriochlorophyll (BChl) c- and a-containing chromosomes from the thermophilic filamentous green photosynthetic bacterium Chloroflexus aurantiacus were investigated using two independent pump-probe techniques with subpicosecond resolution. Isotropic one- and two-color absorption difference experiments using probe wavelengths between 710 and 770 nm reveal BChl c photobleaching (PB) and stimulated emission (SE) decay kinetics with major lifetime components of 50-100 fs, 1-2 ps, and 7-10 ps. Two-color PB.SE profiles pumped at 770 nm and probed at 800 nm (where BChl a pigments absorb) exhibit no detectable rise time. However, two-color experiments using 790 and 820 nm pump and probe wavelengths, respectively, yield PB/SE rise components of 100 fs, 2 ps, and 10 ps. Upon excitation at 720 nm, the BCHl c PB/SE spectrum observed using a broad-band probe continuum displays surprisingly little spectral evolution during the first 2 ps. 65 refs., 13 figs., 3 tabs.