The influence of the FeCp(CO)2+ moiety on the dynamics of the metalloid [Ge9(Si(SiMe3)3)3]- cluster in thf: synthesis and characterization by time-resolved absorption spectroscopy.
The influence of the FeCp(CO)2+ moiety on the dynamics of the metalloid [Ge9(Si(SiMe3)3)3]- cluster in thf: synthesis and characterization by time-resolved absorption spectroscopy.
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DOI：
10.1039/c9dt02091h
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发表时间：
2019-10
影响因子：
4
通讯作者：
N. Michenfelder;C. Gienger;A. Schnepf;A. Unterreiner
中科院分区：
文献类型：
--
作者：
N. Michenfelder;C. Gienger;A. Schnepf;A. Unterreiner
通过盐还原反应成功合成了具有共价键合过渡金属取代基的中性四取代Ge9簇。[Ge9(Si(SiMe3)3)3FeCp(CO)2]的光激发诱导了化合物的激发态动力学，并用扩展宽带fs吸收光谱在紫外-可见-近红外区分析了化合物的激发态动力学。在UV或Vis激发后，电子从[Ge9(Si(SiMe3)3)3]-实体中分离出来，并定位在几百fs内。该簇-电子对的重组发生在大约7- 9ps内。最后，第三个组分可归因于大约150ps内的完全基态恢复。与Li[Ge9(Si(SiMe3)3)3]中的较长寿命组分相比，这要短得多，Li[Ge9(Si(SiMe3)3)3]中的瞬态吸收在紫外激发后超过ns时间尺度。这一观察结果强调了铁元素的强烈影响。
A neutral tetrasubstituted Ge9 cluster with a covalently bound transition metal substituent was synthesized successfully via a salt metathesis reaction. Photoexcitation of [Ge9(Si(SiMe3)3)3FeCp(CO)2] induces excited state dynamics of the compound that was analysed by extended broadband fs absorption spectroscopy in the UV-Vis-NIR region. After UV or Vis excitation, an electron is detached from the [Ge9(Si(SiMe3)3)3]--entity and localizes within few hundred fs. Recombination of this cluster-electron-pair occurs in about 7-9 ps. Finally, a third component can be attributed to complete ground state recovery within roughly 150 ps. This is much shorter compared to a longer-lived component within Li[Ge9(Si(SiMe3)3)3], whose transient absorption exceeds the ns timescale after UV excitation. This observation emphasizes a strong influence of the Fe moiety.