Correlated electron dynamics: how aromaticity can be controlled.
Correlated electron dynamics: how aromaticity can be controlled.
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相关电子动力学：如何控制芳香性。
DOI：
10.1021/ja206193t
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发表时间：
2011
影响因子：
15
通讯作者：
M. Nest
中科院分区：
文献类型：
--
作者：
I. Ulusoy;M. Nest
在这篇文章中，我们证明了可以通过控制电子动力学来关闭分子的芳香性。我们提出了用激光脉冲控制苯的芳香族基态到两个不同的非芳香态的转换。分子波函数的传播采用含时组态相互作用方法。利用最优控制理论对基态和激发态之间的激光脉冲进行了优化。键序和穆利肯电荷是芳香性的标准。非芳香族靶态在碳原子上表现出局域键和部分电荷；这些局域电子在环系中以阿秒时间尺度循环。
In this Article, we show that the aromaticity of a molecule can be turned off by controlling the electron dynamics. We present a controlled switching from the aromatic ground state of benzene to two different nonaromatic states, using a laser pulse. The propagation of the molecular wave function is carried out with the time-dependent configuration interaction method. The laser pulse for switching between the ground and excited states is optimized using optimal control theory. Bond orders and Mulliken charges serve as an aromaticity criterion. The nonaromatic target states exhibit localized bonds and partial charges on the carbon atoms; these localized electrons circulate on an attosecond time scale in the ring system.