Role of initial-state electron correlation in one-photon double ionization of atoms and molecules

Role of initial-state electron correlation in one-photon double ionization of atoms and molecules
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初始态电子关联在​​原子和分子单光子双电离中的作用

DOI:
10.1103/physreva.99.013403
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发表时间:
2019
期刊:
影响因子:
2.9
通讯作者:
McCurdy, C. William
McCurdy, C. William
中科院分区:
物理与天体物理2区
文献类型:
--
作者:
Bello, Roger Y.;Yip, Frank L.;Rescigno, Thomas N.;Lucchese, Robert R.;McCurdy, C. William

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通过将初始态波函数分解为其独特的自然轨道展开,如Löwdin在20世纪50年代定义的并用于现代纠缠研究的那样,我们分析了原子或分子初始态中电子相关在确定单光子双电离角分布中的作用。在精确的数值计算中,两个被射出的电子的终态关联完全被视为He的初态,和是按照自然轨道占用减少的严格顺序从相关构型建立起来的。在双电子原子中,发现初态关联有时起着适度但一般可测量的作用。与此形成鲜明对比的是,对于大量的基态相关组态,产生角分布甚至近似于正确的角分布往往是必要的。取向的单光子双光电离被发现是特别敏感的左右相关沿着键。
By decomposing the initial-state wave function into its unique natural orbital expansion, as defined in the 1950s by Löwdin and used in modern studies of entanglement, we analyze the role of electron correlation in the initial state of an atom or molecule in determining the angular distribution of one-photon double ionization. Final-state correlation of the two ejected electrons is treated completely in numerically accurate calculations as the initial states of He,, andare built up from correlating configurations in strict order of decreasing natural orbital occupations. In the two-electron atoms it is found that the initial-state correlation plays a sometimes modest but generally measurable role. In striking contrast, fora large number of correlating configurations in the ground state is often necessary to produce angular distributions even approximately resembling the correct ones. One-photon double photoionization of orientedis found to be particularly sensitive to left-right correlation along the bond.
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