RUI: Collaborative Research: Multireference Studies of Organic Polyradicals, Radical Reactions and Graphene Nanoribbons

RUI：合作研究：有机多自由基、自由基反应和石墨烯纳米带的多参考研究

• 批准号: 1213271
• 负责人: Carol Parish
• 金额: $ 29万
• 依托单位: University of Richmond
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-08-01 至 2018-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1213271&HistoricalAwards=false
• 关键词: RUI; Collaborative; Research; Multireference; Studies

Carol Parish at the University of Richmond and Hans Lischka at Texas Tech University are supported by an award from the Chemical Theory, Models and Computational methods program to perform theoretical investigations of the structures, reactivities and excited states of di-, tetra- and poly-radical molecules important to understanding reaction mechanisms, pyrolysis and combustion of alternative fuels, anticancer antibiotics and graphene nanodevices. A fundamental understanding of the proper physical characterization of polyradicals is critically important for the further development of multireference (MR) electronic structure theory as well as understanding and controlling chemical phenomenon involving these open-shell intermediates. This proposal focuses on utilizing MR methods (MR-CI, MR-AQCC, CASPT2) to study 1.) model systems such as the geometries and excites states of o-, m- and p-benzyne, 2.) diradical intermediates found in the pyrolyis of asphaltene heteroaromatic compounds, 3.) novel electrocyclization reactions producing diradical intermediates that may function as anticancer antibiotics, 4.) reactions involving tetraradicals and the role that through-bond coupling plays in radical electron interaction, 5.) diradical and multiradical defects in graphene and to benchmark these MR methods against DFT results and 6.) developing input and analysis tools for the COLUMBUS package to facilitate the use of these highly correlated MR methods by the chemical community including undergraduate students.The ability to characterize properly open-shell polyradical species and the corresponding investigation of novel cyclization reactions holds significant promise for advancing the fields of MR theoretical chemistry, mechanistic organic chemistry, materials design and drug optimization. The proposal delineates several carefully conceived theoretical experiments designed to be performed by undergraduate researchers, graduate students and post-baccalaureate or post-doctoral fellows. This will create a community of scientists focusing on the proper characterization of interesting polyradical species using state-of-the-art electronic structure methods. Students at all levels will learn the details of computational quantum mechanics, spectroscopy and methods development.

里士满大学的卡罗尔·帕里什和德克萨斯理工大学的汉斯·利施卡得到了化学理论、模型和计算方法项目的支持，他们对双、四和多自由基分子的结构、反应性和激发态进行理论研究，这些分子对于理解反应机理、替代燃料、抗癌抗生素和石墨烯纳米设备的热解和燃烧非常重要。从根本上理解多自由基的物理特征对于进一步发展多参考(MR)电子结构理论以及理解和控制涉及这些开壳中间体的化学现象是至关重要的。本提案侧重于利用MR方法(MR-CI、MR-AQCC、CASPT2)来研究1。模型体系，如o-，m-和p-Benzyne，2的几何构型和激发态。在沥青质杂芳烃的热解过程中发现的双自由基中间体。产生可用作抗癌抗生素的双自由基中间体的新型电环化反应，4.涉及四种化合物的反应和通键耦合在自由基电子相互作用中所起的作用，5.石墨烯中的双自由基和多自由基缺陷，并将这些磁共振方法与DFT结果和6.为Columbus软件包开发输入和分析工具，以促进包括本科生在内的化学界使用这些高度相关的MR方法。正确表征开壳多自由基物种的能力以及相应的新型环化反应研究对于促进MR理论化学、机械有机化学、材料设计和药物优化领域具有重要的前景。该提案描述了几个精心构思的理论实验，这些实验旨在由本科生研究人员、研究生和学士或博士后研究员进行。这将创建一个科学家社区，专注于使用最先进的电子结构方法正确表征有趣的多自由基物种。所有级别的学生都将学习计算量子力学、光谱学和方法发展的细节。

项目成果

Understanding the Structure and Apo Dynamics of the Functionally Active JIP1 Fragment

了解功能活跃的 JIP1 片段的结构和 Apo 动力学

• DOI: 10.1021/acs.jcim.0c01008
• 发表时间: 2021
• 期刊: Journal of Chemical Information and Modeling
• 影响因子: 5.6
• 作者: Ojaghlou, Neda;Airas, Justin;McRae, Lauren M.;Taylor, Cooper A.;Miller, Bill R.;Parish, Carol A.
• 通讯作者: Parish, Carol A.

Diastereoselective synthesis of new Thiazolyl-Indazole derivatives from R-carvone: A combined experimental and theoretical study

R-香芹酮非对映选择性合成新型噻唑基吲唑衍生物：实验与理论相结合的研究

• DOI: 10.1016/j.tet.2020.131830
• 发表时间: 2021
• 期刊: Tetrahedron
• 影响因子: 2.1
• 作者: N’Ait Ousidi, A.;Itto, M.Y. Ait;Auhmani, A.;Loubidi, M.;Riahi, A.;Daran, J.-C.;Esseffar, M.;Parish, Carol A.
• 通讯作者: Parish, Carol A.

Isofunctional Clustering and Conformational Analysis of the Arsenate Reductase Superfamily Reveals Nine Distinct Clusters

• DOI: 10.1021/acs.biochem.0c00651
• 发表时间: 2020-11-10
• 期刊: BIOCHEMISTRY
• 影响因子: 2.9
• 作者: Rosen，Mikaela R.;Leuthaeuser，Janelle B.;Fetrow，Jacquelyn S.
• 通讯作者: Fetrow，Jacquelyn S.