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Femtosecond phase of charge separation in reaction centers of Chloroflexus aurantiacus

机译:绿屈挠弯曲反应中心的电荷分离飞秒相

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摘要

Difference absorption spectroscopy with temporal resolution of 20 fsec was used to study the primary phase of charge separation in isolated reaction centers (RCs) of Chloroflexus aurantiacus at 90 K. An ensemble of difference (light-minus-dark) absorption spectra in the 730-795 nm region measured at -0.1 to 4 psec delays relative to the excitation pulse was analyzed. Comparison with analogous data for RCs of HM182L mutant of Rhodobacter sphaeroides having the same pigment composition identified the 785 nm absorption band as the band of bacteriopheophytin ΦB in the B-branch. By study the bleaching of this absorption band due to formation of ΦB-, it was found that a coherent electron transfer from P* to the B-branch occurs with a very small delay of 10-20 fsec after excitation of dimer bacteriochlorophyll P. Only at 120 fsec delay electron transfer from P* to the A-branch occurs with the formation of bacteriochlorophyll anion BA- absorption band at 1028 nm and the appearance of P* stimulated emission at 940 nm, as also occurs in native RCs of Rb. sphaeroides. It is concluded that a nuclear wave packet motion on the potential energy surface of P* after a 20-fsec light pulse excitation leads to the coherent formation of the P+ΦB- and P+BA- states. PUBLICATION ABSTRACT)
机译:使用时间分辨力为20 fsec的差吸收光谱技术研究了90 K时金绿假单胞菌孤立反应中心(RCs)中电荷分离的主要相。730-C中的差(光-暗-暗)吸收光谱集合分析了相对于激发脉冲在-0.1至4皮秒延迟处测得的795 nm区域。与具有相同颜料组成的球形红细菌红球菌HM182L突变体的RCs的类似数据进行比较,将785 nm吸收带确定为B分支中的细菌脱镁叶绿素ΦB。通过研究由于形成ΦB-而导致的该吸收带的漂白,发现在激发二聚体叶绿素P后,从P *到B分支的相干电子转移发生了非常小的延迟,即10-20 fsec。在120 fsec的延迟下,发生了从P *到A分支的电子转移,在1028 nm处形成了细菌叶绿素阴离子BA-吸收带,并在940 nm处出现了P *激发的发射,这也发生在Rb的天然RC中。球菌。结论是,在20 fsec的光脉冲激发之后,P *的势能表面上的核波包运动导致P +ΦB-和P + BA-状态的相干形成。出版物摘要)

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