Intensity borrowing via excitonic couplings among Soret and Qy transitions of bacteriochlorophylls in the pigment aggregates of chlorosomes, the light-harvesting antennae of green sulfur bacteria

Yutaka Shibata, Shingo Tateishi, Shosuke Nakabayashi, Shigeru Itoh, Hitoshi Tamiaki

研究成果: Article査読

22 被引用数 (Scopus)

抄録

Model calculations of linear dichroism (LD) and circular dichroism (CD) spectra were conducted for the chlorosomes of green sulfur bacteria, Chlorobium phaeobacteroides and Chlorobium tepidum, on the basis of the theory of delocalized exciton. The chlorosomes of Chl. phaeobacteroides and Chl. tepidum contain bacteriochlorophylls (BChls) e and c as the major light-harvesting pigments, respectively. The excitonic couplings among the Soret and Q y transitions were considered on the basis of the "rodlike" structural model for the pigment self-aggregates in a chlorosome. Trial simulations were conducted by assuming the Bx and By transition-dipole vectors to be parallel to the molecular x- and y-axes, respectively. The simulation at this stage could nicely reproduce the larger splitting of the Soret band and more significant enhancement of the Q y band upon formation of chlorosome in the BChl e-containing chlorosome than in the BChl c-containing one. Intensity borrowing was indicated to be the key mechanism inducing the enhancement of the Qy band in the BChl e-containing chlorosomes. However, the simulated LD and CD spectra in the Soret region showed qualitative disagreement from the observed ones. To resolve the deviations, the directions of the Bx and By transition-dipole vectors and the orientations of the molecular planes of BChls were adjusted in the next stage. The fine-tuning of these parameters resulted in a striking agreement between the observed and simulated CD and LD spectra over the whole spectral range studied. The best fit was obtained when the B x and By transition-dipole vectors were assumed to be rotated 25° clockwise from the molecular x- and y-axes and the molecular planes in the pigment aggregate were tilted 5° from that assumed in the original model without alteration in the direction of the molecular y-axis. The calculated spectral profiles were affected little by the change in the curvatures of the rod surface, showing that the optical spectra of chlorosomes were determined essentially by the local pigment arrangement, but not by the higher-order structure, of the aggregate.

本文言語English
ページ(範囲)7504-7515
ページ数12
ジャーナルBiochemistry
49
35
DOI
出版ステータスPublished - 2010 9 7
外部発表はい

ASJC Scopus subject areas

  • 生化学

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