The charge-transfer properties of the S2 state of fucoxanthin in solution and in fucoxanthin chlorophyll-a/c2 protein (FCP) based on stark spectroscopy and molecular-orbital theory.

The Journal of Physical Chemistry. B
Lavanya PremvardhanRienk van Grondelle

Abstract

Fucoxanthin chlorophyll-a/c 2 protein (FCP), the membrane-intrinsic light harvesting complex from the diatom Cyclotella meneghiniana, is characterized by Stark spectroscopy to obtain a quantitative measure of the excited-state dipolar properties of the constituent pigments. The electro-optical properties of the carotenoid fucoxanthin (Fx), the primary light harvester in FCP, were determined from the Stark spectrum measured in a MeTHF glass (77 K) and compared to the results from electronic-structure calculations. On photon absorption by Fx, a 17 D change in the static dipole moment (|Delta mu|exp), and a somewhat larger |Delta mu|exp at the red edge, are measured for the S 0 --> S 2 (1 (1)A g (-)-like -->1 (1)B u *+-like) transition. The large change in dipole moment indicates that Fx undergoes photoinduced charge transfer (CT), and underscores the influence of the S 2 state on the polarity-dependent excited-state dynamics of Fx that has so far been attributed to, and discussed in terms of, the S 0 and the S 1/ICT states. MNDO-PSDCI and SACCI-CISD calculations indicate that the 1 (1)B u (*+)-like state intrinsically possesses a dipole moment much smaller than the 2 (1)A g (*-)-like state, suggesting that solvent fields promote ...Continue Reading

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Citations

Oct 15, 2011·Photosynthesis Research·Ritsuko FujiiHideki Hashimoto
Jun 28, 2012·The Journal of Organic Chemistry·Christian BrücknerRobert R Birge
Jan 22, 2013·The Journal of Physical Chemistry. a·Ronald L ChristensenRobert R Birge
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Sep 20, 2012·The Journal of Physical Chemistry Letters·D KosumiH Hashimoto

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