Cui Mengnan, Reuter Karsten, Margraf Johannes T
Fritz Haber Institute of the Max Planck Society, 14195 Berlin, Germany.
University of Bayreuth, Bavarian Center for Battery Technology (BayBatt), 95448 Bayreuth, Germany.
J Chem Theory Comput. 2024 Jun 25;20(12):5276-5290. doi: 10.1021/acs.jctc.4c00228. Epub 2024 Jun 12.
The density functional tight-binding (DFTB) approach allows electronic structure-based simulations at length and time scales far beyond what is possible with first-principles methods. This is achieved by using minimal basis sets and empirical approximations. Unfortunately, the sparse availability of parameters across the periodic table is a significant barrier to the use of DFTB in many cases. We therefore propose a workflow that allows the robust and consistent parametrization of DFTB across the periodic table. Importantly, our approach requires no element-pairwise parameters so that the parameters can be used for all element combinations and are readily extendable. This is achieved by parametrizing all elements on a consistent set of artificial homoelemental crystals, spanning a wide range of coordination environments. The transferability of the resulting periodic table baseline parameters to multielement systems and unknown structures is explored and the model is extensively benchmarked against previous specialized and general DFTB parametrizations.
密度泛函紧束缚（DFTB）方法能够在长度和时间尺度上进行基于电子结构的模拟，这远远超出了第一性原理方法所能达到的范围。这是通过使用最小基组和经验近似来实现的。不幸的是，在许多情况下，整个周期表中参数的稀疏可用性是使用DFTB的一个重大障碍。因此，我们提出了一种工作流程，该流程能够在整个周期表上对DFTB进行稳健且一致的参数化。重要的是，我们的方法不需要元素对参数，这样参数就可以用于所有元素组合，并且易于扩展。这是通过在一组一致的人工同素晶体上对所有元素进行参数化来实现的，这些晶体涵盖了广泛的配位环境。我们探索了所得周期表基线参数对多元素系统和未知结构的可转移性，并将该模型与先前的专门和通用DFTB参数化进行了广泛的基准测试。
