Melkozernov Alexander N, Bibby Thomas S, Lin Su, Barber James, Blankenship Robert E
Department of Chemistry and Biochemistry and Center for the Study of Early Events in Photosynthesis, Arizona State University, Tempe, Arizona 85287-1604, USA.
Biochemistry. 2003 Apr 8;42(13):3893-903. doi: 10.1021/bi026987u.
Excitation energy transfer and trapping processes in an iron stress-induced supercomplex of photosystem I from the cyanobacterium Synechocystis sp. PCC6803 were studied by time-resolved absorption and fluorescence spectroscopy on femtosecond and picosecond time scales. The data provide evidence that the energy transfer dynamics of the CP43'-PSI supercomplex are consistent with energy transfer processes that occur in the Chl a network of the PSI trimer antenna. The most significant absorbance changes in the CP43'-PSI supercomplex are observed within the first several picoseconds after the excitation into the spectral region of CP43' absorption (665 nm). The difference time-resolved spectra (DeltaDeltaA) resulting from subtraction of the PSI trimer kinetic data from the CP43'-PSI supercomplex data indicate three energy transfer processes with time constants of 0.2, 1.7, and 10 ps. The 0.2 ps kinetic phase is tentatively interpreted as arising from energy transfer processes originating within or between the CP43' complexes. The 1.7 ps phase is interpreted as possibly arising from energy transfer from the CP43' ring to the PSI trimer via closely located clusters of Chl a in CP43' and the PSI core, while the slower 10 ps process might reflect the overall excitation transfer from the CP43' ring to the PSI trimer. These three fast kinetic phases are followed by a 40 ps overall excitation decay in the supercomplex, in contrast to a 25 ps overall decay observed in the trimer complex without CP43'. Excitation of Chl a in both the CP43'-PSI antenna supercomplex and the PSI trimer completely decays within 100 ps, resulting in the formation of P700(+). The data indicate that there is a rapid and efficient energy transfer between the outer antenna ring and the PSI reaction center complex.
利用飞秒和皮秒时间尺度的时间分辨吸收光谱和荧光光谱,研究了来自集胞藻6803(Synechocystis sp. PCC6803)的铁胁迫诱导的光系统I超复合物中的激发能量转移和俘获过程。数据表明,CP43'-PSI超复合物的能量转移动力学与PSI三聚体天线的叶绿素a网络中发生的能量转移过程一致。在激发进入CP43'吸收光谱区域(665 nm)后的最初几个皮秒内,观察到CP43'-PSI超复合物中最显著的吸光度变化。从CP43'-PSI超复合物数据中减去PSI三聚体动力学数据得到的差分时间分辨光谱(DeltaDeltaA)表明存在三个时间常数分别为0.2、1.7和10 ps的能量转移过程。0.2 ps的动力学相初步解释为源于CP43'复合物内部或之间的能量转移过程。1.7 ps的相可能解释为能量从CP43'环通过CP43'和PSI核心中紧密相邻的叶绿素a簇转移到PSI三聚体,而较慢的10 ps过程可能反映了从CP43'环到PSI三聚体的整体激发转移。这三个快速动力学相之后是超复合物中40 ps的整体激发衰减,相比之下,在没有CP43'的三聚体复合物中观察到的整体衰减为25 ps。CP43'-PSI天线超复合物和PSI三聚体中的叶绿素a激发在100 ps内完全衰减,导致形成P700(+)。数据表明,外天线环和PSI反应中心复合物之间存在快速而有效的能量转移。