T. Pullerits et al., EXCITON DELOCALIZATION LENGTH IN THE B850 ANTENNA OF RHODOBACTER-SPHAEROIDES, Journal of physical chemistry, 100(25), 1996, pp. 10787-10792
The properties of elementary excited states in the B850 band of the pe
ripheral light-harvesting antenna (LH2) of the photosynthetic purple b
acterium Rhodobacter sphaeroides has been studied at room temperature
by means of femtosecond transient absorption experiments combined with
computer simulations. Polarized pump-probe kinetics have a fast compo
nent of 100 and 65 fs for the anisotropic and isotropic decays, respec
tively. Direct numerical simulations show that for incoherent hopping-
like excitation transfer in the B850 ring of 18 Bchl a molecules at ro
om temperature the fast component of the anisotropy decay is 3 times l
onger than the corresponding component of the isotropic decay, strongl
y suggesting that delocalized exciton states are involved in the obser
ved dynamics. To estimate the coherence length of the exciton we have
measured absorption difference spectra of LH2 from 810 to 880 nm 2 ps
after the excitation into the B800 band with 75 fs laser pulses. Excit
on calculations where also monomeric doubly excited states are include
d give a good fit to the experimental spectra for a coherence length o
f 4 +/- 2 bacteriochlorophyll monomers. The relatively big error limit
s are due to the lack of detailed enough information about the doubly
excited state of Bchl a.