title: Spectral heterogeneity and time-resolved spectroscopy of excitation energy transfer in membranes of Heliobacillus mobilis at low temperatures.
abstract: Transient absorption difference spectra in the Qy absorption band from membranes of Heliobacillus mobilis were recorded at 140 and 20 K upon 200 fs laser pulse excitation at 590 nm. Excitation transfer from short wavelength absorbing forms of bacteriochlorophyll g to long wavelength bacteriochlorophyll g occurred within 1-2 ps at both long wavelength bacteriochlorophyll g occurred within 1-2 ps at both temperatures. In addition, a slower energy transfer process with a time constant of 15 ps was observed at 20 K within the pool of long wavelength-absorbing bacteriochlorophyll g. Energy transfer from long wavelength antenna pigments to the primary electron donor P798 was observed, yielding the primary charge-separated state P798+A0-. The time constant for this process was 30 ps at 140 K and about 70 ps at 20 K. A decay component with smaller amplitude and a lifetime of up to hundreds of picoseconds was observed that was centered around 814 nm at 20 K. Kinetic simulations using simple lattice models reproduce the observed decay kinetics at 295 and 140 K, but not at 20 K. The kinetics of energy redistribution within the spectrally heterogeneous antenna system at low temperature argue against a simple "funnel" model for the organization of the antenna of Heliobacillus mobilis and favor a more random spatial distribution of spectral forms. However, the relatively high rate of energy transfer from long wavelength antenna bacteriochlorophyll g to the primary electron donor P798 at low temperature is difficult to explain with either of these models.
authors.affiliation: Department of Chemistry and Biochemistry, Arizona State University, Tempe 85287-1604.
authors.forename: S
authors.initials: S
authors.lastname: Lin
authors.forename: F A
authors.initials: FA
authors.lastname: Kleinherenbrink
authors.forename: H C
authors.initials: HC
authors.lastname: Chiou
authors.forename: R E
authors.initials: RE
authors.lastname: Blankenship
mesh_terms: D001419:Bacteria / Q000737:chemistry* / Q000528:radiation effects; D001429:Bacteriochlorophylls / Q000737:chemistry / Q000528:radiation effects; D055592:Biophysical Phenomena; D001703:Biophysics; D004735:Energy Transfer; D007700:Kinetics; D045342:Light-Harvesting Protein Complexes; D008566:Membranes / Q000737:chemistry / Q000528:radiation effects; D008956:Models, Chemical; D010777:Photochemistry; D010788:Photosynthesis; D045322:Photosynthetic Reaction Center Complex Proteins / Q000737:chemistry / Q000528:radiation effects; D013053:Spectrophotometry; D013696:Temperature
chemical_list: D001429:Bacteriochlorophylls; D045342:Light-Harvesting Protein Complexes; D045322:Photosynthetic Reaction Center Complex Proteins