Excitation energy transfer and exciton annihilation in the
isolated B800−850 antenna complex from the purple
bacterium Rhodopseudomans acidophila (strain 10050) were
studied by one-color transient absorption
experiments with a typical pulse length of 50 fs at room temperature
and 77 K. The anisotropy kinetics
observed within the B800 band are clearly wavelength dependent,
indicating that the B800 ↔ B800 energy
transfer or excitonic relaxation processes are wavelength dependent.
The depolarization times found at room
temperature were 400 fs at 790 nm, 820 fs at 800 nm, and 360 fs at 810
nm. A faster depolarization time
of 240 fs was obtained at 801 nm at 77 K, which is suggested to
originate from excitonic relaxation. Energy
transfer from the B800 to the B850 occurs in ∼0.8 ps at room
temperature and ∼1.30 ps at 77 K. The
kinetics obtained within the B800 band were observed for the first time
to exhibit a dramatic dependence on
the excitation intensity. When the excitation intensity is higher
than 1.09 × 1014 photons
pulse-1 cm-2,
the
transient absorption kinetics after ∼3 ps are dominated by a
long-lived bleaching. However, in contrast, a
slowly recovering excited-state absorption was found to be dominant at
lower pump intensities. This intensity
dependence is attributed to the variation of the population
distribution between the lowest and next higher
lying excitonic levels of the B850 ring, a result of exciton
annihilation in the lowest-state, following the rapid
energy transfer from the B800 to the B850 band and subsequent fast
excitonic relaxation within the excitonic
manifold of the B850 ring. The time constant for this annihilation
process was found to be ∼1 ps. Excitonic
calculations indicate that several high-lying excitonic states show
good spectral overlap with the B800 band,
and thus, they could serve as excellent acceptors for the energy
transfer from B800 to B850.