Computational Ultrafast X-ray Science

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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.