Computational Ultrafast X-ray Science

计算超快 X 射线科学

• 批准号: RGPIN-2020-06444
• 负责人: Schuurman, Michael
• 金额: $ 2.62万
• 依托单位: University of Ottawa
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=748204
• 关键词: Computational; Ultrafast; ray; Science

This proposal aims to develop a computational toolkit for the simulation of time-resolved X-ray spectroscopies. There are three main research thrusts in this proposal that focus on important aspects of this problem for which the existing theoretical and computational techniques are insufficient to describe ultrafast processes in the X-ray domain for complex molecules in condensed phases. In particular, this proposal will: 1.) develop computational approaches that can quantitatively describe the electronic structure of core-excitation processes, particularly from valence excited states, 2.)  development quantum chemistry based approaches to simulate the observable spectroscopic signatures of these dynamical and chemical processes in condensed phases, an advantage of working in the X-ray energy regime, and 3.) simulate the underlying molecular dynamics, which requires that one couple an ab initio description of the chemical processes of interest to the role of the environment (i.e. solvent) in facilitating particular reactive outcomes. This last component will generally require novel methods in linking modern quantum chemical approaches for determining the relevant potential energy surfaces to approaches in direct quantum dynamics. It is anticipated that the work in this proposal will be characterized by close collaboration with experimental researchers at Canadian and international institutions who are both employing and developing time-resolved X-ray spectroscopic techniques. The close coupling of theory and experiment is a hallmark of my research program and the now-established network of leading-edge experimental collaborators in this field represents a significant scientific asset that will enable the successful implementation of this research program.

该提案旨在开发一个用于模拟时间分辨 X 射线光谱的计算工具包。该提案有三个主要研究重点，重点关注这一问题的重要方面，而现有的理论和计算技术不足以描述超快。特别是，该提案将：1.）开发定量描述核心激发过程的电子结构的计算方法，特别是价激发态的电子结构，2.）开发基于量子化学的方法来模拟凝聚相中这些动力学和化学过程的可观察光谱特征，这是在 X 射线能量范围内工作的优势，以及 3.) 模拟潜在的分子动力学，这需要一对夫妇从头描述环境（即溶剂）在促进特定反应结果中的作用的化学过程，这最后一个组成部分通常需要将现代量子化学方法与直接确定相关势能表面的方法联系起来的新方法。预计该提案中的工作将与加拿大和国际机构的实验研究人员密切合作，这些机构正在采用和开发时间分辨 X 射线光谱技术。我的研究计划的标志以及现已在该领域建立的前沿实验合作者网络代表了一项重要的科学资产，将使该研究计划的成功实施。