Theory of Dynamical Correlated-Electron Processes in Molecules Induced and Probed with x-Ray Light

X 射线诱导和探测的分子动态关联电子过程理论

• 批准号: 2207656
• 负责人: Francois Mauger
• 金额: $ 15万
• 依托单位: Louisiana State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-09-01 至 2025-08-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2207656&HistoricalAwards=false
• 关键词: Theory; Dynamical; Correlated; Electron; Processes

X-ray free-electron laser (XFEL) light sources are opening avenues to observe the motion of electrons inside matter with unprecedented space and time resolution. By accessing core levels, x-ray pulses can discriminatively interrogate different atoms in molecules, and they can do so with femtosecond (one millionth of a billionth of a second) resolution or faster, reaching the natural scales at which electrons move in these systems. This project will study a range of time-dependent correlated-electron processes in organic molecules that can be induced and probed with x-rays. To do so, the PI and his group will leverage existing quantum-chemistry packages to simulate the interaction between x-rays and molecules. While theoretical, this project will aim to identify processes and observables that are accessible to measurements, with the ultimate objective to collaborate with XFEL experimental campaigns. The project will serve the national interest through the advancement of x-ray-enabled molecular science and through the development of human resources via the training of junior researchers at the undergraduate and graduate levels.The PI and his group will study the interactions between molecules and x-ray light, as the vehicle for triggering and observing time-dependent correlated processes in these systems, with an emphasis on core electrons. Of the two main objectives, one will be to routinely simulate a range of correlated processes in organic molecules that can be induced and/or probed with x-rays. To do so, simulations will use an explicit treatment of electron correlation in a multi-reference complete- or restricted-active space formal-ism (MR-CAS/RAS) using density-functional-theory, or otherwise optimized, molecular orbitals to improve the convergence of the MR-CAS/RAS. An additional objective of the project will be to uniquely connect the correlated dynamics and processes observed in these simulations, i.e., the wave functions, to observables that are accessible to experiments. This project will also investigate some of the practical aspects of modeling light-matter interactions with realistic XFEL pulses.This project is jointly funded by the Atomic, Molecular, and Optical Physics Theory Program and the Established Program to Stimulate Competitive Research (EPSCoR).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.

X射线自由电子激光（XFEL）光源正在开放途径，以观察到具有前所未有的空间和时间分辨率的电子内部的运动。通过获得核心水平，X射线脉冲可以区分分子中的不同原子，并且可以通过秒秒（十亿分之一的一百万秒）分辨率或更快地进行分辨率，从而达到电子在这些系统中移动的自然尺度。该项目将研究有机分子中的一系列时间依赖性相关 - 电子过程，这些过程可以用X射线诱导和探测。为此，PI和他的小组将利用现有的量子化学套件来模拟X射线与分子之间的相互作用。虽然理论上，该项目将旨在确定可访问测量值的过程和可观察到的物品，并具有与XFEL实验活动合作的最终目标。 The project will serve the national interest through the advancement of x-r​​ay-enabled molecular science and through the development of human resources via the training of junior researchers at the undergraduate and graduate levels.The PI and his group will study the interactions between molecules and x-ray light, as the vehicle for triggering and observing time-dependent correlated processes in these systems, with an emphasis on core electrons.在这两个主要目标中，将定期模拟可以用X射线诱导和/或探测的有机分子中的一系列相关过程。为此，模拟将使用密度功能理论或其他优化的分子轨道来改善MR-CAS/RAS的收敛性。该项目的另一个目标是将在这些模拟（即波函数）中观察到的相关动力学和过程唯一连接到实验可访问的可观察物。该项目还将调查建模与现实XFEL脉冲的光线相互作用的一些实际方面。该项目由原子，分子和光学物理学理论计划和既定的竞争性研究（EPSCOR）共同资助，以反映NSF的法定任务，并通过评估构成的范围及其范围的范围，这是由Infectiral and Intelliqu and Intelliqu and Intelliqu and Internial and Infectial and Infectial and Intperiatial。