Long-range intermolecular charge transfer induced by laser pulses: an explicitly time-dependent configuration interaction approach.
Long-range intermolecular charge transfer induced by laser pulses: an explicitly time-dependent configuration interaction approach.
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激光脉冲引起的长程分子间电荷转移：一种明确的时间依赖性构型相互作用方法。
DOI：
10.1039/b817873a
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发表时间：
2009
期刊：
影响因子：
--
通讯作者：
P. Saalfrank
中科院分区：
文献类型：
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作者：
Stefan Klinkusch;T. Klamroth;P. Saalfrank
在本文中，我们报告了通过瞬态构型相互作用单粒子（TD-CIS）方法模拟激光驱动的多电子动力学。该方法能够超越微扰理论明确地描述与时间相关的现象，并且可以系统地改进。与大多数时间相关的密度泛函方法相比，它还允许我们正确处理长程电荷转移状态。例如，通过 TD-CIS 研究了供体（乙烯）和受体分子（四氰乙烯，TCNE）之间的激光脉冲诱导电荷转移。此外，还考虑由多个供体和/或受体组成的较大聚集体。结果表明，所研究系统的电荷分布和偶极矩可以通过（一系列）激光脉冲进行切换，这些激光脉冲会诱导选择性的状态到状态的电子跃迁。
In this paper, we report simulations of laser-driven many-electron dynamics by means of the time-dependent configuration interaction singles (TD-CIS) approach. The method is capable of describing explicitly time-dependent phenomena beyond perturbation theory and is systematically improvable. In contrast to most time-dependent density functional methods it also allows us to treat long-range charge-transfer states properly. As an example, the laser-pulse induced charge transfer between a donor (ethylene) and an acceptor molecule (tetracyanoethylene, TCNE) is studied by means of TD-CIS. Also, larger aggregates consisting of several donors and/or acceptors are considered. It is shown that the charge distribution and hence the dipole moments of the systems under study are switchable by (a series of) laser pulses which induce selective, state-to-state electronic transitions.