RUI: Double Photoionization to Probe Electron Correlation Many-Electron Molecules

电子关联是一种重要的物理现象，它对物质的行为和结构有着重要的影响。 几十年的研究已经导致了最简单的原子和分子中电子动力学的精确解释方法，并阐明了在纯双电子系统中单个光子喷射两个电子的影响。这个项目的目标是研究具有两个以上电子的基本分子中的相关电子动力学。这项工作将推进理解这一过程的基础科学，这是目前最完整的纯双电子分子，化学相关的物种，如乙烯和水。相关电子相互作用是原子水平上物质组织和结构的基础，并且对于研究和更好地理解仍然至关重要。更全面地了解具有两个以上电子的分子中的电子相关性的更广泛的后果将影响许多其他研究领域，包括化学，原子和分子物理学，分子生物学和材料科学。涉及第二行原子的分子的双光电离（DPI）是理论的长期目标，并且这项工作寻求推进这些能力，特别是通过符合动量成像光谱学来支持最近的实验观察（例如，COLTRIMS）测量乙烯和水分子的双电离，其可以通过库仑爆炸后的离子碎片的运动学上完整的重建来观察体框架角分布。这两种分子目标提供了一个显着更复杂的分子，以比较新的理论计算与这些测量的水平，目前存在的H2。用光子从一个原子或分子中移去两个电子，必然需要对电子相关性的正确描述，并作为对这种现象的直接探测。发展和扩展的理论计算致力于双电离先前用于研究这一过程中最简单的分子，H2和最近的锂，将扩大到考虑多电子多原子分子作为目标，为了更好地理解更广泛的后果电子相关的基本分子含有第二行原子拥有更多的电子。 更全面地理解和详细描述高度相关的电子动力学效应，特别是在连续介质中，是原子和分子物理研究界的长期目标。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的知识价值和更广泛的影响审查标准进行评估来支持。

Electron correlation is a fundamental phenomena which greatly impacts the behavior and structure of all matter. Many decades of research have led to accurate ways of accounting for the dynamics of electrons in the simplest atoms and molecules and have elucidated the impacts of ejecting two electrons by a single photon in purely two electron systems. The goal of this project is to examine the correlated electron dynamics within fundamental molecules with more than two electrons. This work will advance the basic science of understanding this process, which is currently most complete in purely two-electron molecules, to chemically relevant species, e.g. ethylene and water. Correlated electron interactions are fundamental to the organization and structure of matter at the atomic level and continue to be of vital importance to study and better understand. Broader consequences of a more complete understanding of electron correlation in molecules with more than two electrons would impact many other fields of study, including chemistry, atomic and molecular physics, molecular biology, and material science. Double photoionization (DPI) of molecules involving second-row atoms is a long-term goal of theory and this work seeks to advance these capabilities, in particular to support recent experimental observations via coincidence momentum imaging spectroscopy (e.g., COLTRIMS) measuring the double ionization of ethylene and water molecules that can observe the body-frame angular distributions via a kinematically complete reconstruction of the ionic fragments after Coulomb explosion. Both molecular targets provide a significantly more complicated molecule to compare new theoretical calculations with these measurements at the level of what presently exists for H2. The removal of two electrons from an atom or molecule by photon(s) necessarily requires a correct description of electron correlation and serves as a direct probe of this phenomenon. The development and expansion of theoretical calculations dedicated to double ionization previously employed for studying this process in the simplest molecule, H2 and most recently Li2, will be expanded to consider multi-electron polyatomic molecules as targets, in order to better understand the broader consequences of electron correlation in fundamental molecules containing second-row atoms possessing many more electrons. A fuller understanding and detailed description of the effects of highly correlated electron dynamics, particularly in the continuum, is a long-term goal of the atomic and molecular physics research community.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.