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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Interference in acetylene intersystem crossing acts as the molecular analog of Young's double-slit experiment
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Interference in acetylene intersystem crossing acts as the molecular analog of Young's double-slit experiment

机译：乙炔系统间交叉的干扰是杨氏双缝实验的分子类似物

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摘要

We report on an experimental approach that reveals crucial details of the composition of singlet-triplet mixed eigenstates in acetylene. Intersystem crossing in this prototypical polyatomic molecule embodies the mixing of the lowest excited singlet state (S_1) with 3 triplet states (T_1, T_2, and T_3). Using high-energy (157-nm) photons from an F_2 laser to record excited-state photoelectron spectra, we have decomposed the mixed eigenstates into their S_1, T_3, T_2, and T_1 constituent parts. One example of the interpretive power that ensues from the selective sensitivity of the experiment to the individual electronic state characters is the discovery and examination of destructive interference between two doorway-mediated intersystem crossing pathways. This observation of an interference effect in nonradiative decay opens up possibilities for rational coherent control over molecular excited state dynamics.
机译：我们报告了一种实验方法，该方法揭示了乙炔中单重态-三重态混合本征态组成的关键细节。该原型多原子分子的系统间交叉体现了最低激发单重态（S_1）与3个三重态（T_1，T_2和T_3）的混合。使用来自F_2激光器的高能（157 nm）光子来记录激发态光电子能谱，我们将混合的本征态分解为S_1，T_3，T_2和T_1的组成部分。从实验对单个电子状态特征的选择性敏感性中获得的解释力的一个例子是发现和检查两个门道介导的系统间交叉途径之间的破坏性干扰。这种对非辐射衰变中干扰效应的观察为分子激发态动力学的合理相干控制开辟了可能性。

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