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首页> 外文期刊>The Journal of Chemical Physics >Recovering dynamic correlation in spin flip configuration interaction through a difference dedicated approach
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Recovering dynamic correlation in spin flip configuration interaction through a difference dedicated approach

机译：通过差异专用方法恢复自旋翻转配置交互中的动态相关性

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This article introduces the restricted-active-space n-spin flip configuration interaction models, RAS(S)-SF and RAS(S, 2h, 2p)-SF, which provide highly correlated, yet low cost approaches for treating polyradical systems. These levels of theory add electronic degrees of freedom beyond those of previous spin flip approaches in order to achieve accurate ground and excited state energetics. The effects of additional dynamic correlation were investigated by comparing these two techniques to the prior RAS(h, p)-SF method on a variety of test systems, including multiple electronic states of methylene, tetramethyleneethane, three binuclear transition metal complexes, and a tetracene dimer. RAS(S, 2h, 2p)-SF significantly improves state descriptions in all cases and provides high accuracy even when using a minimal number of spin flips. Furthermore, this correlated level of theory is shown to be extensible to the large systems involved in singlet fission, where the multi-excitonic states in tetracene dimers are difficult to simulate with standard methods and therefore are still a matter of debate. Using a triple-zeta basis, the double triplet state, 1(TT), is predicted to be unbound. This result contradicts lower levels of theory and provides important insight into tetracene's ability to undergo efficient singlet fission. Published by AIP Publishing.
机译：本文介绍了限制 - 有效空间N-Xpip配置交互模型，RAS（S）-SF和RA（S，2H，2P）-SF，其提供高度相关的，但低成本的处理热大道系统。这些理论水平增加了超出了先前自旋触发器方法的电子自由度，以实现准确的地面和激励状态能量学。通过将这两种技术与各种测试系统的预先RAS（H，P）-SF方法进行比较，包括多种电子状态，包括多种电子状态的亚甲基，四甲基乙烷，三个核核过渡金属配合物和四烯来研究额外动态相关的影响。二聚体。 RAS（S，2H，2P）-SF在所有情况下显着提高了状态描述，即使使用最小数量的旋转翻转时，也能提供高精度。此外，这种相关水平的理论水平被证明是对偏出裂变中涉及的大型系统的可伸展，其中难以使用标准方法模拟四烯二聚体中的多激子状态，因此仍然是争论的问题。使用Triple-Zeta基础，预计Double Triplet状态为1（TT）是未绑定的。这一结果与较低的理论水平矛盾，并为四烯经过高效单线裂变的能力提供了重要的洞察。通过AIP发布发布。

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