CAREER: Quantum Chemistry for Predicting and Quantifying Photoinduced Nonadiabatic Dynamics

宾夕法尼亚大学的约瑟夫·苏博特尼克得到了化学系理论、模型和计算方法计划的支持，以开发量子化学中专门用于模拟非绝热动力学过程的新方法。特别是，苏博特尼克教授和他的研究小组正在追求三个不同的目标：1.最大限度地减少状态间耦合的非绝热状态的新公式，并为理解非绝热跃迁提供最佳基础；2.计算激发态能量和波函数响应性质的新算法，特别是使用局部关联技术和其他可应用于大系统的计算廉价技术；3.提出了产生和分析绝热和非绝热导数耦合的新方法，重点研究了它们的动力学性质(包括电子动量)。所有上述电子结构理论中的技术都是模拟光致非绝热动力学的必要工具。这项研究将在光化学和能量科学领域产生广泛的影响，特别是在电子和能量转移方面。目前，现代太阳能研究的重点是捕捉太阳光发电，我们迫切需要工具来预测新材料，以最大限度地提高太阳能电池的效率。这项研究提案将为未来的应用提供许多这样的工具。苏博特尼克还将参加本科生水星计算化学大会，以便与本科生研究人员建立联系，教他们如何开发量子化学软件包，这样他们也可以在这个新兴领域做出贡献。

Joseph Subotnik of the University of Pennsylvania is supported by an award from the Theory, Models and Computational Methods program in the Chemistry division to develop new methods in quantum chemistry specifically to be used for modeling nonadiabatic dynamical processes.In particular, Professor Subotnik and his research group are pursuing three different goals: 1. New formulations for diabatic states to minimize inter-state coupling and provide an optimal basis for understanding nonadiabatic transitions;2. Novel algorithms to compute excited state energies and wave function response properties, specifically using local correlation techniques and other omputationally inexpensive techniques applicable to big systems; 3. New approaches to produce and analyze derivative couplings between adiabatic and diabatic states, with a heavy focus on their their dynamical properties (including electronic momentum).All of the techniques above in electronic structure theory are necessary tools for modeling photo-induced nonadiabatic dynamics.This research will have a broad impact in the field of photochemistry and energy science, especially with regards to electron and energy transfer. Currently, modern research in solar energy focuses on capturing sun light to produce electricity, and we urgently need tools to predict new materials for maximizing the efficiency of solar cells. This research proposal will provide many of those tools for future applications. Subotnik will also participate in the undergraduate MERCURY conference for computational chemistry, in order to connect with undergraduate researchers and teach them how to develop quantum chemistry packages, so they can also make contributions in this emerging field.