- 作者: A. G. Yakovleva and V. A. Shuvalova,b
- 中文摘要: Formation of a nuclear wavepacket on the potential energy surface of the primary electron donor P* induced by 30-fs excitation of pheophytin-modified Rhodobacter sphaeroides R-26 reaction centers leads to a reversible and irreversible appearance of the state P+BA- monitored by the measurements of the 1020-nm band which is characteristic of the radical anion band of bacteriochlorophyll monomer BA-. The reversible appearance of the state P+BA- is characterized by two (130 and 320 cm-1) vibration modes and related to the creation of maximal value of the Franck-Condon factor when the wavepacket is near an intersection of the P* and P+BA- potential energy surfaces. The irreversible formation of the state P+BA- with a time constant of 3 ps is accompanied by oscillations with frequencies of 9 and 33 cm-1. These results show that the nuclear vibration modes (9 and 33 cm-1) on the P* potential energy surface have near their bottom the intersection with the P+BA- surface as well. The electron transfer time between P* and BA was estimated to be in the range of 700 fs. This is larger than the wavepacket intersection time for the 130 cm-1 mode (~100 fs) and comparable with that for the 33 cm-1 mode (~600 fs). Therefore the reversible electron transfer with small amplitude can be observed for the 130 cm-1 mode, while the irreversible one is allowed for the 33 cm-1 mode that is probably important for the primary charge separation.
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