Shaper-based photoelectron tomography of free electron wave packets from multiphoton ionization with tailored 3D laser fields

利用定制 3D 激光场对来自多光子电离的自由电子波包进行基于整形器的光电子断层扫描

• 批准号: 467215508
• 负责人: Professor Dr. Matthias Wollenhaupt
• 金额: --
• 依托单位: Arbeitsgruppe Ultraschnelle Kohärente Dynamik
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/467215508?language=en
• 关键词: Shaper; based; photoelectron; tomography; free

In this proposal, we suggest an experimental method for generating fully controlled and tailored three-dimensional (3D) ultrashort laser light fields. The 3D field is created in the focus of two polarization-shaped femtosecond laser beams propagating at an angle in different directions. In recent theoretical studies, these so-called “super-chiral” light fields have been shown provide exceptionally high sensitivity for distinguishing enantiomers. The main goal of our project is to experimentally explore the new possibilities offered by tailored 3D light fields for coherent control of atomic and molecular photoionization dynamics. In the proposed experiment, we investigate the multiphoton ionization (MPI) of atoms and chiral molecules with these fully controlled 3D laser fields by measuring the 3D photoelectron momentum distributions (PMD) of the released free electron wave packets. Because our established waveplate-based photoelectron tomography technique is not applicable to 3D fields, we introduce a novel pulse shaper-based photoelectron tomography method to accurately measure and reconstruct the full 3D PMDs. In our experiments, MPI serves as a model system to analyze the physical mechanisms of coherent control of ultrafast dynamics driven by 3D fields. At the same time, this method is used as a very sensitive nonlinear method for in-situ characterization of these 3D fields. We demonstrate the novelty of our approach by discussing various MPI scenarios and showing the corresponding simulated 3D PMDs which are only accessible by these 3D fields. We validate the simulation method by comparison with our previous experimental results.In the proposed project, we combine our expertise in advanced supercontinuum polarization pulse shaping, high-precision photoelectron tomography, and theoretical modeling of coherent control of atomic and molecular dynamics. Our central goal is the experimental generation and control of unprecedented 3D PMDs using 3D fields. Tailored 3D fields open new prospects for the control of light-induced ultrafast processes, not only in coherent control, but also in many areas of atomic, molecular, and optical physics such as chiral recognition, laser spectroscopy, nonlinear microscopy, laser chemistry, quantum information, and materials processing, to name a few.

在本提案中，我们提出了一种生成完全受控和定制的三维 (3D) 超短激光场的实验方法。3D 场是在以不同方向传播的两束偏振形飞秒激光束的焦点处创建的。在最近的理论研究中，这些所谓的“超手性”光场已被证明可以为区分对映体提供极高的灵敏度。我们项目的主要目标是通过实验探索定制的 3D 光场为区分对映体提供的新可能性。在所提出的实验中，我们通过测量释放的自由电子波的 3D 光电子动量分布 (PMD)，研究了使用这些完全控制的 3D 激光场的原子和手性分子的多光子电离 (MPI)。由于我们建立的基于波片的光电子断层扫描技术不适用于 3D 领域，因此我们引入了一种新颖的基于脉冲整形器的光电子断层扫描方法来精确测量和重建完整的数据包。在我们的实验中，MPI 作为模型系统来分析 3D 场驱动的超快动力学相干控制的物理机制，同时该方法被用作一种非常灵敏的非线性方法，用于现场表征。我们通过讨论各种 MPI 场景并展示只能通过这些 3D 场访问的相应模拟 3D PMD，展示了我们方法的新颖性。我们通过与之前的实验结果进行比较来验证模拟方法。在拟议的项目中，我们结合了先进的超连续偏振脉冲整形、高精度光电子断层扫描以及原子和分子动力学相干控制的理论建模方面的专业知识，我们的中心目标是使用 3D 场实验生成和控制前所未有的 3D PMD。定制的 3D 场为光致超快过程的控制开辟了新的前景，不仅在相干区域控制方面，而且在许多原子、分子和光学物理领域，如手性识别、激光光谱学、非线性显微镜、激光化学、量子信息和材料加工等等。