Further development of internally contracted multi-reference coupled-cluster theory

内契约多参考耦合簇理论的进一步发展

• 批准号: 201645791
• 负责人: Professor Dr. Andreas Köhn
• 金额: --
• 依托单位: Institut für Theoretische Chemie (ITheoC)
• 依托单位国家: 德国
• 项目类别: Research Grants
• 财政年份: 2011
• 资助国家: 德国
• 起止时间: 2010-12-31 至 2021-12-31
• 项目状态: 已结题
• 来源: https://gepris.dfg.de/gepris/projekt/201645791?language=en
• 关键词: Further; development; internally; contracted; multi

Accurate first-principles methods are an important building block of modern quantum chemistry. They may serve for the reliable prediction of energies and properties of transient species or hazardous compounds and provide an internal standard for more approximate methods. The internally-contracted multireference coupled-cluster (icMRCC) theory developed by the applicant promises to transfer the high accuracy of standard coupled-cluster theory to systems with complex electronic structure, like polyradicals and transition metal compounds with open d-shells. In this project, we want to further improve the methodological foundations of the icMRCC theory and provide a new and efficient implementation that allows to take full advantage of the potential of the method. Specific developments are the investigation of pragmatic approximations to the full-blown icMRCC theory and a multistate extension, allowing to treat arbitrary excited states and quasi-degenerate cases. By using an embedding method that will also be further developed during this project, we will be able to apply the newly developed methods to large molecules, for instance, to realistic models for computing the energetics at reaction centers of catalysts or magnetic couplings of molecular magnets.

精确的第一性原理方法是现代量子化学的重要组成部分。它们可用于瞬态物种或有害化合物的能量和性质的可靠预测，并为更近似的方法提供内标。由申请人开发的内部收缩多参考耦合簇（icMRCC）理论承诺将标准耦合簇理论的高精度转移到具有复杂电子结构的系统，如具有开放d-壳层的多自由基和过渡金属化合物。在这个项目中，我们希望进一步改进icMRCC理论的方法论基础，并提供一种新的有效的实现，以充分利用该方法的潜力。具体的发展是调查实用的近似成熟的icMRCC理论和多态扩展，允许治疗任意激发态和准退化的情况下。通过使用在本项目中也将进一步开发的嵌入方法，我们将能够将新开发的方法应用于大分子，例如，用于计算催化剂反应中心或分子磁体磁耦合的能量学的现实模型。

项目成果

Improved and simplified orthogonalisation scheme and connected triples correction within the internally contracted multireference coupled-cluster method

内部契约多参考耦合聚类方法中改进和简化的正交化方案和连接三元组校正

• DOI: 10.1080/00268976.2020.1743889
• 发表时间: 2020
• 期刊: Molecular Physics
• 影响因子: 1.7
• 作者: A. Köhn;J. A. Black;Y. A. Aoto;M. Hanauer
• 通讯作者: M. Hanauer

A generalized hybrid scheme for multireference methods.

多参考方法的广义混合方案

• DOI: 10.1063/5.0067511
• 发表时间: 2021
• 期刊: The Journal of chemical physics
• 作者: A. Waigum;J. A. Black;A. Köhn
• 通讯作者: A. Köhn