International Collaboration in Chemistry: New First Principles Methods for Nonadiabatic Dynamics

斯坦福大学的托德马丁内斯在化学系化学理论、模型和计算方法的支持下，与英国利兹大学的德米特里·沙拉希林进行合作研究。 这是一个国际化学合作组织（ICC）的提案。 Shalashilin博士的研究得到了EPSRC的支持。PI及其研究小组正在开发和应用新的基于轨迹的方法来描述量子力学动力学。这些方法与从头算分子动力学方法兼容，即势能面和非绝热耦合可以用量子化学技术在飞行中计算。 目前正在探讨两种方法（多配置Escherfest和多产卵），以确定每种方法的优点，以便将它们结合起来，发挥各自的优势。这项工作产生的新方法将在AIMS-MolPro代码中实施，并提供给广泛的研究人员。PI将研究使用图形处理单元（GPU）来加速动力学计算。 该项目为新一代精确的第一原理动力学方法提供了基础，这些方法可以结合量子力学效应，例如多个电子状态之间的非绝热表面交叉和轻核（如质子）的隧穿。这些方法对化学，特别是光化学有着广泛的影响。这些方法也将有助于解释超快时间分辨泵浦-探测光谱。该项目涉及利兹和斯坦福大学之间的学生交流（短期停留最多一个月），从而为参与的研究生提供有关每个国家学术环境的扩展视野。国际科学与工程办公室为该奖项提供联合资助。

Todd Martinez of Stanford University is supported by the Chemical Theory, Models and Computational Methods in the Chemistry Division to engage in collaborative research with Dmitry Shalashilin of the University of Leeds in the UK. This is an International Collaborations in Chemistry (ICC) proposal. Dr. Shalashilin's research is supported by the EPSRC. The PIs and their research groups are developing and applying new trajectory based methods for describing quantum mechanical dynamics. These methods are compatible with ab initio molecular dynamics methods, i.e. the potential energy surfaces and nonadiabatic couplings can be computed on the fly with quantum chemical techniques. Two such methods (multi-configurational Ehrenfest and multiple spawning) are being explored in order to determine the advantages of each so that they may be combined in a way which leverages their respective advantages. The new methodology that emerges from this work will be implemented in the AIMS-MolPro code and made available to a wide range of researchers. The PIs will investigate the use of graphical processing units (GPUs) to accelerate the dynamics calculations. The project provides a foundation for a new generation of accurate first principles dynamics methods that can incorporate quantum mechanical effects such as nonadiabatic surface crossing between multiple electronic states and tunneling of light nuclei such as protons. Such methods have a broad impact on chemistry, especially photochemistry. These methods will also be useful for interpreting ultrafast time-resolved pump-probe spectra. The project involves interchange (for short stays up to a month) of students between Leeds and Stanford, thus providing the involved graduate students with an expanded vista concerning the academic environment in each countryThe Office of International Science and Engineering provides co-funding for this award.