Molecular Free Electron Vortices in Photoionization by Polarization-Tailored Ultrashort Laser Pulses.
Molecular Free Electron Vortices in Photoionization by Polarization-Tailored Ultrashort Laser Pulses.
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DOI：
10.3389/fchem.2022.899461
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发表时间：
2022
影响因子：
5.5
通讯作者：
中科院分区：
文献类型：
--
作者：
原子和分子自由电子涡旋（FEVs）以其螺旋形的动量分布为特征，由于其多变的形状和不寻常的拓扑性质，近年来引起了人们的广泛关注。不久后，他们的理论预测的单光子电离（SPI）的He原子使用对反向旋转的圆偏振阿秒脉冲，FEV已被实验证明的多光子电离（MPI）的碱金属原子使用单色和双色圆偏振飞秒脉冲序列。最近，我们报道了一个基于含时薛定谔方程（TDSE）从头算解的数值模型，对二维原子与偏振成形超短激光场相互作用的实验结果进行了分析。在这里，我们应用二维TDSE模型来研究分子FEV创建的SPI和MPI的双原子分子使用偏振定制的单色和双色飞秒脉冲序列。我们研究了电子-核耦合动力学对涡旋形成动力学的影响，并讨论了CEP平均和转动平均对光电子动量分布的影响。通过分析分子结构和动力学是如何在光电子螺旋中留下印记的，我们探索了分子FEVs用于超快光谱的潜力。
Atomic and molecular free electron vortices (FEVs), characterized by their spiral-shaped momentum distribution, have recently attracted a great deal of attention due to their varied shapes and their unusual topological properties. Shortly after their theoretical prediction by the single-photon ionization (SPI) of He atoms using pairs of counterrotating circularly polarized attosecond pulses, FEVs have been demonstrated experimentally by the multiphoton ionization (MPI) of alkali atoms using single-color and bichromatic circularly polarized femtosecond pulse sequences. Recently, we reported on the analysis of the experimental results employing a numerical model based on the ab initio solution of the time-dependent Schrödinger equation (TDSE) for a two-dimensional (2D) atom interacting with a polarization-shaped ultrashort laser field. Here, we apply the 2D TDSE model to study molecular FEVs created by SPI and MPI of a diatomic molecule using polarization-tailored single-color and bichromatic femtosecond pulse sequences. We investigate the influence of the coupled electron-nuclear dynamics on the vortex formation dynamics and discuss the effect of CEP- and rotational averaging on the photoelectron momentum distribution. By analyzing how the molecular structure and dynamics is imprinted in the photoelectron spirals, we explore the potential of molecular FEVs for ultrafast spectroscopy.
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DOI：
10.1063/1.4996816
发表时间：
2017-11
期刊：
Structural dynamics (Melville, N.Y.)
影响因子：
--
作者：
Bircher MP;Liberatore E;Browning NJ;Brickel S;Hofmann C;Patoz A;Unke OT;Zimmermann T;Chergui M;Hamm P;Keller U;Meuwly M;Woerner HJ;Vaníček J;Rothlisberger U
通讯作者：
Rothlisberger U
影响因子：
8.6
作者：
Djiokap, J. M. Ngoko;Hu, S. X.;Starace, Anthony F.
通讯作者：
Starace, Anthony F.
影响因子：
8.6
作者：
Bian, Xue-Bin;Bandrauk, Andre D.
通讯作者：
Bandrauk, Andre D.
影响因子：
3.3
作者：
Becker, Wilhelm;Milosevic, Dejan B.
通讯作者：
Milosevic, Dejan B.
影响因子：
2.9
作者：
Djiokap, J. M. Ngoko;Starace, Anthony F.
通讯作者：
Starace, Anthony F.