CAREER: New Methods for Dynamical Quantum Chemistry

犹他大学的Ryan Steele获得了化学学部化学理论模型和计算方法项目的奖励，以开发化学过程计算模拟的新方法。目前，这种模拟显示出揭示与社会相关的化学挑战的关键细节的潜力，包括可再生能源。然而，它们也受到计算成本障碍的阻碍，这限制了这些方法的适用性。该研究计划寻求替代方法，这些方法极大地扩展了这些方法的适用性范围，并开发了新的模拟方法。具体来说，这项工作将解决分子的运动和这种运动决定化学反应的方式。在这个项目中开发的计算工具将提供给更广泛的研究界。与这些发展相一致，该计划的综合教育组成部分通过使用新开发的模拟/可视化工具和教学法，努力改善学生和教育者看待化学的方式——从字面上和概念上。这些教育目标将促进教学法的变革，并增加服务不足的学生及其教育工作者获得教育的机会。提出的关键方法——也是这个资助期研究的独特方面——是一个新的算法接口，它将从头算电子结构理论与采样和动态动力学结合在一起。这项工作旨在利用电子结构方法内部工作的固有空间和时间可分离性，用于大型反应性化学系统的新动态特定模拟。应用于水氧化配合物，其中独特的电子结构和核运动丰富，将使这种新的方法。

Ryan Steele of the University of Utah is supported by an award from the Chemical Theory Models and Computational Methods program in the Chemistry Division to develop new approaches to the computational simulation of chemical processes. Such simulations currently exhibit the potential to unravel critical details of societally relevant chemistry challenges, including renewable energy. They also, however, are impeded by computational cost hurdles which limit the applicability of these methods. This research program seeks alternative approaches which dramatically extend the range of applicability of these methods and the development of new simulation methodology. Specifically, this work will address the motion of molecules and the manner in which this motion dictates chemical reactivity. The computational tools developed in this project will be made available to the broader research community. In concert with these developments, integrated education components of this program strive to improve the manner in which students and educators view chemistry -- both literally and conceptually -- by using newly developed simulation/visualization tools and pedagogy. These education aims will facilitate a change in pedagogy, as well as increase access for underserved students and their educators.The key proposed methodology -- and the unique aspect of the research in this funding period -- is a new algorithmic interface which marries ab initio electronic structure theory with sampling and on-the-fly dynamics. This work seeks to exploit the inherent spatial and temporal separability of the inner workings of electronic structure methods for new, dynamics-specific simulations of large, reactive chemical systems. Application to water oxidation complexes, where unique electronic structure and nuclear motion abound, will be enabled by this new methodology.