Coherent Control of the Photoionization of Pyrazine

Coherent Control of the Photoionization of Pyrazine
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吡嗪光电离的相干控制

DOI:
10.1021/jz301144q
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发表时间:
2012-10
影响因子:
5.7
通讯作者:
Gordon, Robert J.
Gordon, Robert J.
中科院分区:
化学2区
文献类型:
--
作者:
Hu, Zhan;Singha, Sima;Zhao, Youbo;Barry, Grant E.;Seideman, Tamar;Gordon, Robert J.

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大多数通过量子力学干涉控制共振光吸收的尝试都局限于具有特定状态配置和选择规则的原子和小分子。在这里,我们用实验说明了在复杂的分子系统中产生激光诱导的双折射的可能性。我们的方法利用了多原子分子的非绝热激发态动力学特性。具体而言,我们表明,它是可能的,以构建飞秒脉冲使用遗传算法来抑制电离的孤立吡嗪分子在预先指定的时间。这些数据表明,透明性是通过在耦合的S1/S2势能表面的区域中定位波包来实现的,在该区域中,向离子状态的垂直过渡在能量上是被禁止的。这种方法是通用的,并且不需要分子哈密顿量的先验知识。光谱学、光化学和激发态
Most attempts to control the absorption of resonant light by quantum mechanical interference have been limited to atoms and small molecules with specialized state configurations and selection rules. Here we illustrate experimentally the possibility of creating laser-induced transparencies in complex molecular systems. Our approach takes advantage of the nonadiabatic excited-state dynamics characteristic of polyatomic molecules. Specifically, we show that it is possible to construct femtosecond pulses using a genetic algorithm to suppress the ionization of isolated pyrazine molecules at a prespecified time. The data suggest that transparency is achieved by localization of a wave packet in a region of the coupled S1/S2 potential energy surfaces, where a vertical transition to the ionic state is energetically forbidden. This approach is general and does not require prior knowledge of the molecular Hamiltonian. SECTION: Spectroscopy, Photochemistry, and Excited States
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