CAREER: New Methods for Dynamical Quantum Chemistry

犹他州大学的Ryan Steele获得了化学系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。 这种模拟目前显示出揭示社会相关化学挑战的关键细节的潜力，包括可再生能源。 然而，它们也受到限制这些方法的适用性的计算成本障碍的阻碍。 这项研究计划寻求替代方法，大大扩展了这些方法的适用范围和新的模拟方法的发展。 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性的方式。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努力改善学生和教育工作者通过使用新开发的模拟/可视化工具和教学法从字面上和概念上看待化学的方式。 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的机会。关键的拟议方法-以及在此资助期间研究的独特方面-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结合在一起。 这项工作旨在利用电子结构方法的内部工作的内在空间和时间的可分离性，用于大型反应性化学系统的新的动态特定模拟。 这种新的方法将使水氧化复合物，独特的电子结构和核运动丰富的应用。

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.