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

电子关联是一种对所有物质的行为和结构产生重大影响的基本现象。几十年的研究已经导致了准确的方法来解释最简单的原子和分子中的电子动力学，并阐明了在纯两个电子系统中由单个光子抛出两个电子的影响。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关联电子动力学。这项工作将推动理解这一过程的基础科学，这一过程目前在纯两电子分子中最完整，到化学上相关的物种，如乙烯和水。相关的电子相互作用是物质在原子水平上的组织和结构的基础，对于研究和更好地理解它仍然是至关重要的。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、分子生物学和材料科学。涉及第二排原子的分子的双光电离(DPI)是一个长期的理论目标，这项工作试图提高这些能力，特别是支持最近通过符合动量成像谱(例如COLTRIMS)测量乙烯和水分子的双电离的实验观测，该光谱可以通过动态地重建库仑爆炸后的离子碎片来观察身体-框架的角分布。这两个分子靶都提供了一个明显更复杂的分子，以便在现有的H2水平上将新的理论计算与这些测量进行比较。用光子从原子或分子中移走两个电子(S)必然需要对电子关联的正确描述，并作为这一现象的直接探针。以前用于研究最简单的分子H2和最近的Li2中的双电离过程的理论计算的发展和扩展，将扩展到将多电子多原子分子作为目标，以便更好地理解包含拥有更多电子的第二排原子的基本分子中电子关联的更广泛结果。更全面地了解和详细描述高度关联的电子动力学的影响，特别是在连续体中的影响，是原子和分子物理研究界的长期目标。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

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.