Molecular-Frame Photoelectron Angular Distributions of CO in the Vicinity of Feshbach Resonances: An XCHEM Approach,Journal of Chemical Theory and Computation

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Molecular-Frame Photoelectron Angular Distributions of CO in the Vicinity of Feshbach Resonances: An XCHEM Approach
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2021-09-16 , DOI: 10.1021/acs.jctc.1c00480
Vicent J Borràs ₁ , Jesús González-Vázquez ₁ , Luca Argenti ₂ , Fernando Martín _{1,

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Affiliation

The advent of ultrashort XUV pulses is pushing for the development of accurate theoretical calculations to describe ionization of molecules in regions where electron correlation plays a significant role. Here, we present an extension of the XCHEM methodology to evaluate laboratory- and molecular-frame photoelectron angular distributions in the region where Feshbach resonances are expected to appear. The performance of the method is demonstrated in the CO molecule, for which information on Feshbach resonances is very scarce. We show that photoelectron angular distributions are dramatically affected by the presence of resonances, to the point that they can completely reverse the preferred electron emission direction observed in direct nonresonant photoionization. This is the consequence of significant changes in the electronic structure of the molecule when resonances decay, an effect that is mostly driven by electron correlation in the ionization continuum. The present methodology can thus be helpful for the interpretation of angularly resolved photoionization time delays in this and more complex molecules.

中文翻译：

Feshbach 共振附近 CO 的分子框架光电子角分布：XCHEM 方法

超短 XUV 脉冲的出现推动了精确理论计算的发展，以描述电子相关性发挥重要作用的区域中分子的电离。在这里，我们提出了 XCHEM 方法的扩展，以评估预计出现 Feshbach 共振的区域中的实验室和分子框架光电子角分布。该方法的性能在 CO 分子中得到证明，关于 Feshbach 共振的信息非常稀少。我们表明，共振的存在会显着影响光电子角分布，以至于它们可以完全逆转在直接非共振光电离中观察到的首选电子发射方向。这是共振衰减时分子电子结构发生显着变化的结果，这种效应主要由电离连续谱中的电子相关性驱动。因此，本方法有助于解释这种和更复杂分子中角度分辨的光电离时间延迟。

更新日期：2021-10-12

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