FEMTOSECOND AND HOLE-BURNING STUDIES OF B800S EXCITATION-ENERGY RELAXATION DYNAMICS IN THE LH2 ANTENNA COMPLEX OF RHODOPSEUDOMONAS-ACIDOPHILA (STRAIN-10050)
Hm. Wu et al., FEMTOSECOND AND HOLE-BURNING STUDIES OF B800S EXCITATION-ENERGY RELAXATION DYNAMICS IN THE LH2 ANTENNA COMPLEX OF RHODOPSEUDOMONAS-ACIDOPHILA (STRAIN-10050), Journal of physical chemistry, 100(29), 1996, pp. 12022-12033
One- and two-color pump/probe femtosecond and hole-burning data are re
ported for the isolated B800-850 (LH2) antenna complex of Rhodopseudom
onas acidophila (strain 10050). The two-color profiles are interpretab
le in terms of essentially monophasic B800-->B850 energy transfer with
kinetics ranging from 1.6 to 1.1 ps between 19 and 130 K for excitati
on at or to the red of the B800 absorption maximum. The B800 zero-phon
on hole profiles obtained at 4.2 K with burn frequencies located near
or to the red of this maximum yielded a transfer time of 1.8 ps. B800
hole-burning data (4.2 K) are also reported for chromatophores at ambi
ent pressure and pressures of 270 and 375 MPa. At ambient pressure the
B800-B850 energy gap is 950 cm(-1), while at 270 snd 375 MPa it is cl
ose to 1000 and 1050 cm(-1), respectively. However, no dependence of t
he B800-->B850 transfer time on pressure was observed, consistent with
data for the B800-850 complex of Rhodobacter sphaeroides. The resilie
nce of the transfer rate to pressure-induced changes in the energy gap
and the weak temperature dependence of the rare are consistent with t
he model that has the spectral overlap (of Forster theory) provided by
the B800 fluorescence origin band and weak vibronic absorption bands
of B850. However, both the time domain and hole-burning data establish
that there is an additional relaxation channel for B800, which is obs
erved when excitation is located to the blue of the B800 absorption ma
ximum. Several explanations fur this faster channel are considered, in
cluding that it is due to intra-B800 energy transfer or a manifestatio
n of coupling of B800 with quasi-degenerate upper exciton levels of th
e B850 molecules. The data indicate that it is not due to vibrational
relaxation.