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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Solvent Polarity Dependence of Photoinduced Charge Separation and Recombination Processes of Ferrocene-C_(60) Dyads
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Solvent Polarity Dependence of Photoinduced Charge Separation and Recombination Processes of Ferrocene-C_(60) Dyads

机译：二茂铁-C_（60）染料的光诱导电荷分离和复合过程的溶剂极性依赖性

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摘要

Photoinduced charge-separation and charge-recombination processes of the three ferrocene-C_(60) dyads have been investigated by using laser flash photolysis methods. From molecular orbital calculations, the HOMO states are delocalized over the ferrocene and linking phenyl-ethenyl group connecting ferrocene and C_(60), while the LUMO states are on C_(60). From short fluorescence lifetimes (≤ 120 ps) of the fullerene moieties of the dyads, charge separations were suggested. Charge-separated states in the dyads were observed upon femtosecond laser irradiation. The rate constants for the charge separation were on the order of 10~(10) s~(-1), and the quantum yields were close to unity in various solvents, such as benzonitrile, anisole, and toluene. It was confirmed that the absorption bands of the radical cation moiety shifted to longer wavelength side in polar solvents, probably due to structural change in the charge-separated states. The lifetimes of the charge-separated states of the dyads with longer linkage became longer, up to several 10s of nanoseconds in less polar solvents, while the lifetimes in polar solvents were shorter, since the charge-recombination processes are in the Marcus "inverted region". On the other hand, the lifetime of the charge-separated state in the dyad with an acetyl linking group was on the order of nanoseconds in all of the solvents because of fast charge recombination of shorter distance. It was confirmed that the charge-recombination process generated the ground state of the dyads predominantly.
机译：利用激光闪光光解方法研究了三种二茂铁-C_（60）二元化合物的光诱导电荷分离和电荷重组过程。从分子轨道计算来看，HOMO态在二茂铁上是离域的，并且连接二茂铁和C_（60）的连接苯基-乙烯基，而LUMO态在C_（60）上。从二聚体的富勒烯部分的短荧光寿命（≤120 ps）开始，建议进行电荷分离。在飞秒激光照射下观察到二元组中的电荷分离状态。电荷分离的速率常数约为10〜（10）s〜（-1），在各种溶剂（如苯甲腈，苯甲醚和甲苯）中，量子产率接近于1。证实了在阳离子溶剂中自由基阳离子部分的吸收带移至更长的波长侧，这可能是由于电荷分离态的结构变化所致。具有较长键合的二元体的电荷分离态的寿命变得更长，在极性较小的溶剂中可达数十纳秒，而极性溶剂的寿命则较短，因为电荷重组过程位于马库斯“倒置区” ”。另一方面，由于较短距离的快速电荷重组，在所有溶剂中，具有乙酰基连接基团的二元体系中电荷分离态的寿命约为纳秒。证实了电荷复合过程主要产生了二重基态。

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