CAREER: SusChEM: Computational Studies of Light-Induced Dynamics in First-Row Transition Metal Complexes

在这个由化学部化学结构、动力学机制B计划资助的CAREER项目中，州立大学北卡罗来纳州化学系的Elena Jakubikova教授研究了以地球上丰富的金属为基础的过渡金属络合物如何与光相互作用。该项目的目标是利用计算机建模来更深入地了解此类复合物的结构-性质关系，以便可以设计新的发色团，光催化剂或光磁材料。该项目位于计算，无机和物理化学的接口，因此能够很好地将计算化学作为一种有价值的工具介绍给高中，本科和研究生阶段的广泛学生。收藏的染料在马克斯A。韦弗染料图书馆在北卡罗来纳州州立大学是用来激励高中和本科生的研究和教育活动。 学生们为图书馆开发了一套数据，用于计算可见吸收光谱的基准计算方法，并筛选染料用作染料敏化太阳能电池中的发色团。基于第一行过渡金属络合物的发色团和光催化剂的合理设计依赖于这些络合物如何吸收和耗散光的基础知识。特别是，了解非辐射衰变过程的机制，如内部转换和系统间交叉，是我们控制这些系统的激发态特性的能力的关键。本项目的目标是从理论上更好地理解第一行过渡金属配合物的非辐射衰变机制，以便更合理地开发基于地球丰富金属的高效发色团，光催化剂和光磁材料。具体而言，该项目侧重于促进铁基复合物中超快系统间交叉事件的结构因素。该项目涉及一系列八面体以及低配位铁配合物的计算研究，利用密度泛函理论，含时密度泛函理论，非绝热过渡态理论，和非绝热表面跳跃动力学。 少数民族和经济困难的学生通过与NC项目SEED计划和NSF-研究经验的本科生计划在化学系现有的关系招募。 当地高中教师提供的工具和专业知识，开发和实施自己的计算化学模块到先进的安置化学课程使用北卡罗来纳州高中计算化学服务器。

In this CAREER project funded by the Chemical Structure, Dynamics & Mechanism B Program of the Chemistry Division, Professor Elena Jakubikova of the Department of Chemistry at North Carolina State University investigates how transition metal complexes based on earth-abundant metals interact with light. The goal of this project is to utilize computer modeling to obtain a deeper understanding of structure-property relationships in such complexes, so that new chromophores, photocatalysts or photomagnetic materials may be designed. The project lies at the interface of computational, inorganic, and physical chemistry, and is therefore well positioned to introduce computational chemistry as a valuable tool to a wide range of students at the high school, undergraduate and graduate levels. Collection of dyes in the Max A. Weaver Dye Library at North Carolina State University is used to motivate the research and educational activities of high school and undergraduate students. The students contribute developing a set of data for the library to benchmark computational methodologies for calculations of visible absorption spectra and to screen dyes for use as chromophores in dye-sensitized solar cells.The rational design of chromophores and photocatalysts based on first row transition metal complexes relies on the fundamental knowledge of how these complexes absorb and dissipate light. In particular, understanding the mechanisms of nonradiative decay processes, such as internal conversion and intersystem crossing, is key to our ability to control excited state properties of these systems. The goal of this project is to obtain a better theoretical understanding of the mechanism of nonradiative decay in first row transition metal complexes, so that a more rational approach to the development of efficient chromophores, photocatalysts, and photomagnetic materials based on earth-abundant metals can be taken. Specifically, the project focuses on structural factors that facilitate the ultrafast intersystem crossing events in iron-based complexes. The project involves computational studies on a series of octahedral as well as low coordinate iron complexes utilizing density functional theory, time-dependent density functional theory, nonadiabatic transition state theory, and nonadiabatic surface hopping dynamics. Minority and economically disadvantaged students are recruited through the existingrelationships with the NC Project SEED program and the NSF-Research Experiences for Undergraduates Program in the Department of Chemistry. Local high school teachers are provided with the tools and expertiseto develop and implement their own computational chemistry modules into the Advanced Placement Chemistry curriculum using the North Carolina High School Computational Chemistry Server.