Experimental and Theoretical Investigations of Organic Reaction Rates and Mechanisms

在这个项目中，由化学系化学结构、动力学和机制 B 项目资助，加州大学洛杉矶分校化学与生物化学系以及化学与生物分子工程系的 K. N. Houk 教授将开发新的计算方法来理解化学反应性、选择性和机制。这项研究涉及物理方程的使用，主要是量子力学和分子动力学。密集的计算机计算可以预测分子的结构以及它们在化学反应过程中转化为产物的过程。 Houk 小组在这一领域处于领先地位，并继续向化学家证明计算是他们实验研究的重要辅助手段。作为该项目的一部分，钙钛矿的计算模型预计将带来新的架构和添加剂，以增强光伏性能。计划的研究将涉及与实验研究小组的广泛合作。这项研究提供了计算基础，有助于更好地理解新的和令人费解的实验结果，并为实验者提供关于新实验的指导。 更广泛影响的活动包括向加州大学洛杉矶分校的学生、高中和公众进行宣传。 小组成员参与对潜在 STEM 学生的外展活动，以吸引他们对计算化学职业的兴奋感。受这笔赠款支持的参与者仍然是加州大学洛杉矶分校科学文化多样性组织 (OCDS) 的活跃成员。Houk 小组率先研究了双峰反应，该反应可以从一个过渡态形成多种产物。这个持续的项目将开发概念来理解有机反应的反应性和机制，并改进定量计算反应速率和机制的计算方法。该项目涉及有机反应（包括溶液中的反应）的反应路径和分子动力学计算。分析反应性的各种方法，例如Houk实验室构思和开发的反应性扭曲/相互作用模型，将应用于有机反应和机制、有机金属反应的选择性以及溶液中反应的分子动力学。将进行新型钙钛矿光伏电池的分析和设计。将开发理解化学反应性的新方法。与实验研究小组在机制和选择性方面的合作有望提供解释并指导未来的研究方向。该项目将有一个重要组成部分致力于新发现的有机和有机金属反应的计算研究。新方法将被开发并与一般化学界共享。新化学的预测将由合作者进行研究。这项研究的更广泛影响包括培训有机计算和理论的未来领导者，教授化学界如何解决计算问题，以及教授理论家如何与实验家沟通。这项研究的高度协作环境对于从事这门科学的研究人员来说是一个显着的好处。本科生、研究生和博士后将接受使用理论和计算的培训，作为解决化学问题的实验的伴侣。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

In this project, funded by the Chemical Structure, Dynamics, and Mechanisms B Program of the Chemistry Division, Professor K. N. Houk of the UCLA Department of Chemistry and Biochemistry, and Chemical and Biomolecular Engineering will develop new computational methods to understand chemical reactivity, selectivity and mechanisms. This research involves the use of equations of physics, primarily quantum mechanics and molecular dynamics. Intensive computer calculations predict the structures of molecules and the processes by which they transform to products during chemical reactions. The Houk group has pioneered in this area and continues to demonstrate to chemists that computation is a crucial adjunct to their experimental research. As one part of this project, computational models for perovskites are expected to lead to new architectures and additives for enhanced photovoltaic performance. Planned research will involve extensive collaboration with experimental research groups. This research provides for computational underpinning and contributes to the better understanding of new and puzzling experimental results, and provides guidance to experimentalists about new experiments. Broader impacts activities include outreach to students at UCLA, high schools and the general public. Group members participate in outreach to potential STEM students to attract them to the excitement of a career in computational chemistry. The participants supported by this grant continue to be active members of the Organization for Cultural Diversity in Science (OCDS) at UCLA.The Houk group has pioneered the study of ambimodal reactions that can form several products from one transition state. This continuing project will develop concepts to understand reactivities and mechanisms for organic reactions, and to improve computational methods for quantitative calculations of reaction rates and mechanisms. This project involves calculations of reaction paths and molecular dynamics of organic reactions, including reactions in solution. Various methods to analyze reactivity, such as the distortion/interaction model of reactivity that was conceived and developed in the Houk lab, will be applied to organic reactions and mechanisms, selectivities of organometallic reactions, and molecular dynamics of reactions in solution. Analyses and design of new perovskite photovoltaics will be performed. New approaches to understanding chemical reactivity will be developed. Collaborations on mechanisms and selectivities with experimental research groups are expected to provide explanations and guide future research directions. This project will have a significant component dedicated to the computational study of newly discovered, organic and organometallic reactions. New methods will be developed and shared with the general chemical community. Predictions of new chemistry will be studied by collaborators. Broader impacts of this research include training of future leaders of organic computation and theory, teaching the chemical community how to solve problems with computation, as well as teaching theoreticians how to communicate with experimentalists. The highly collaborative environment of this research is a significant benefit to the researchers engaged in this science. Undergraduates, graduate students, and postdoctorals will be trained in the use of theory and computation as a companion to experiment for the solution of chemical problems.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.