RUI: Double Photoionization to Probe Electron Correlation in Molecular Targets with more than Two Electrons

电子在原子和分子中的行为是我们理解物质系统的基础。 从将分子结合在一起的基本化学键到宏观物质的整体性质，电子在很大程度上负责液体和固体的化学组成和物理性质。 量子力学已经告诉我们在原子的小尺度上物质的真实性质，但即使是最简单的分子也很难精确表示。 尽管如此，从最基本的层面上研究物质仍然有很多东西要学，包括更好地理解电子相关性的后果，这些后果在很大程度上决定了物质在所有长度尺度上的行为。 电子相关性超越了电子相互排斥的事实;电子不断以基本的方式相互注意，比如自旋相互作用，了解这些相互作用可以更好地告诉我们宇宙的基本结构。 双光电离研究，其中足够能量的光子可以在单个事件中从材料中移除两个电子，直接探测电子相关性。 这项研究将提出精确的方法来描述具有许多电子的分子（如水（H2O））中的双光电离。其目的是更好地理解这些更复杂的目标中的电子相关性，并进一步了解分子中电子的基本相互作用。 该项目将研究具有两个以上电子的简单分子通过单光子电离（双光电离）去除的两个电子的电子相关性，以更好地理解多电子目标受到额外复杂性（H2以外）影响的方式。 从第一原理描述这些事件的理论计算将被应用于具有许多电子的目标，这些电子在光电离事件之前、期间和之后继续与完全相关的电子相互作用。 需要理论支持，以帮助通知和理解最近的实验测量水的双光电离。 希望这个项目能够进一步阐明与分子结合的所有电子如何影响那些将被移动到连续体中的电子的更广泛的后果，以及分子对称性和电子结构的后果如何影响从分子环境中传出的电子。这个奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的评估来支持。影响审查标准。

The behavior of electrons in atoms and molecules is fundamental to our understanding of material systems. From the basic chemical bonds that hold molecules together to the bulk properties of macroscopic matter, electrons are largely responsible for the chemical makeup and physical properties of liquids and solids. Quantum mechanics has informed us of the true nature of matter at the small scale of the atom, but accurately representing even the simplest molecule is challenging. Still, there is much to be learned from studying matter at the most fundamental level, including a better understanding of the consequences of electron correlation that govern so much of how matter behaves at all length scales. Electron correlation goes beyond the fact that electrons repel each other; electrons continually notice each other in fundamental ways, like spin interactions, and learning about those interactions better informs us of the fundamental construction of our universe. Double photoionization studies, where a photon of sufficient energy can remove two electrons from a material in a single event, directly probes electron correlation. This research will advance precise methods to describe double photoionization in molecules with many electrons, like water (H2O). The purpose is to better understand electron correlation in these more-complicated targets and gain further general insights into the fundamental interactions of electrons in molecules. This understanding, once developed, informs multiple technological applications involving chemistry and materials that are essential to a high-tech society.This project will investigate electronic correlation for two electrons removed by single-photon absorptions (double photoionization) for simple molecules with more than two electrons in order to better understand the ways that multi-electron targets are influenced by additional complexity (beyond H2). Theoretical calculations describing these events from first principles will be applied to targets with many electrons that continue to interact with the fully correlated electrons before, during and after the photoionization event. Theoretical support is needed to help inform and understand recent experimental measurements of double photoionization of water. It is hoped that this project can further elucidate the broader consequences of how all of the electrons bound to a molecule can affect those that will be moved into the continuum and how consequences of molecular symmetry and electronic structure impact the outgoing electrons from a molecular environment.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.