Assessment of DFT Methods for Transition Metals with the TMC151 Compilation of Data Sets and Comparison with Accuracies for Main-Group Chemistry
Assessment of DFT Methods for Transition Metals with the TMC151 Compilation of Data Sets and Comparison with Accuracies for Main-Group Chemistry
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DOI：
10.1021/acs.jctc.9b00239
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发表时间：
2019-06-01
影响因子：
5.5
通讯作者：
Kimura, Masanari
中科院分区：
文献类型：
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作者：
Chan, Bun;Gill, Peter M. W.;Kimura, Masanari
在本研究中，我们收集了过渡金属反应的准确参考数据（我们称之为TMC 151），用于评估量子化学方法。它包括双原子离解能和反应能以及典型过渡金属反应的势垒。我们对各种不同类型的DFT方法的评估表明，最准确的泛函包括omega B 97 M-V，omega B 97 X-V，MN 15和B 97 M-rV。值得注意的是，它们之前也被验证为对主族化学具有高度稳健性。然而，即使这些方法显示出过渡金属比主族化学的准确性差得多。对于不太准确的方法，它们对主族和过渡金属化学的准确度之间没有很好的相关性。因此，在开发新的DFT时，评估这两种类型数据的准确性非常重要。在这方面，我们制定了TMC 34模型，用于有效评估过渡金属的性能，这补充了我们先前开发的主族化学MG 8模型。它们共同为新方法的初步评估提供了一种成本效益高的手段。
In the present study, we have gathered a collection (that we term TMC151) of accurate reference data for transition-metal reactions for the assessment of quantum chemistry methods. It comprises diatomic dissociation energies and reaction energies and barriers for prototypical transition-metal reactions. Our assessment of a diverse range of different types of DFT methods shows that the most accurate functionals include omega B97M-V, omega B97X-V, MN15, and B97M-rV. Notably, they have also been previously validated to be highly robust for main-group chemistry. Nevertheless, even these methods show substantially worse accuracies for transition metals than for main-group chemistry. For less accurate methods, there is not a good correlation between their accuracies for main-group and transition-metal chemistries. Thus, in the development of new DFT, it is important to assess the accuracies for both types of data. In this regard, we have formulated the TMC34 model for efficient assessment of the performance for transition metals, which complements our previously developed MG8 model for main-group chemistry. Together, they provide a cost-effective means for initial assessment of new methodologies.