Ultrafast Charge Migration in XUV Photoexcited Phenylalanine: A First-Principles Study Based on Real-Time Nonequilibrium Green’s Functions,The Journal of Physical Chemistry Letters

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Ultrafast Charge Migration in XUV Photoexcited Phenylalanine: A First-Principles Study Based on Real-Time Nonequilibrium Green’s Functions
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-03-01 00:00:00 , DOI: 10.1021/acs.jpclett.8b00025
E. Perfetto _{1,

2} , D. Sangalli ₁ , A. Marini ₁ , G. Stefanucci _{2,

3}

Affiliation

The early-stage density oscillations of the electronic charge in molecules irradiated by an attosecond XUV pulse takes place on femto- or subfemtosecond time scales. This ultrafast charge migration process is a central topic in attoscience because it dictates the relaxation pathways of the molecular structure. A predictive quantum theory of ultrafast charge migration should incorporate the atomistic details of the molecule, electronic correlations, and the multitude of ionization channels activated by the broad-bandwidth XUV pulse. We propose a first-principles nonequilibrium Green’s function method fulfilling all three requirements and apply it to a recent experiment on the photoexcited phenylalanine amino acid. Our results show that dynamical correlations are necessary for a quantitative overall agreement with the experimental data. In particular, we are able to capture the transient oscillations at frequencies 0.15 and 0.30 PHz in the hole density of the amine group as well as their suppression and the concomitant development of a new oscillation at frequency 0.25 PHz after ∼14 fs.

中文翻译：

XUV光激发苯丙氨酸中的超快电荷迁移：基于实时非平衡格林函数的第一性原理研究

阿秒XUV脉冲辐射的分子中的电荷的早期密度振荡发生在飞秒或飞秒级的时间范围内。这种超快速电荷迁移过程是原子科学中的中心主题，因为它决定了分子结构的弛豫途径。超快电荷迁移的预测量子理论应结合分子的原子学细节，电子相关性以及由宽带XUV脉冲激活的多个电离通道。我们提出了满足所有这三个要求的第一性原理非平衡格林函数方法，并将其应用于光激发苯丙氨酸氨基酸的最新实验。我们的结果表明，动力学相关性对于与实验数据进行定量总体吻合是必要的。

更新日期：2018-03-01

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