Structure and Stability of Molecular Crystals with Many-Body Dispersion-Inclusive Density Functional Tight Binding.
Structure and Stability of Molecular Crystals with Many-Body Dispersion-Inclusive Density Functional Tight Binding.
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DOI：
10.1021/acs.jpclett.7b03234
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发表时间：
2018-01
期刊：
影响因子：
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通讯作者：
M. Mortazavi;J. Brandenburg;R. Maurer;A. Tkatchenko
中科院分区：
文献类型：
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作者：
M. Mortazavi;J. Brandenburg;R. Maurer;A. Tkatchenko
准确预测分子晶体的结构和稳定性在材料科学中是至关重要的，并且需要可靠的远程色散相互作用模型。半经验电子结构方法在计算上比从头算方法的计算效率更高，从而使结构采样具有显著的加速比。我们通过基于电荷布居的方法将Tkatchenko-Scheffler van der Waals方法(TS)和多体色散方法(MBD)与三阶密度泛函紧束缚(DFTB3)相结合。我们发现X23分子晶体基准数据库总体上表现良好，尽管对晶体体积的低估可以追溯到DFTB参数化。我们在包含VDW的DFTB3结构上使用DFT+MBD能量学实现了精确的晶格能量预测，与完全DFT处理相比，加速比高达3000倍。这表明包含VDW的DFTB3可以作为一种可行的结构预筛选工具用于晶体结构预测。
Accurate prediction of structure and stability of molecular crystals is crucial in materials science and requires reliable modeling of long-range dispersion interactions. Semiempirical electronic structure methods are computationally more efficient than their ab initio counterparts, allowing structure sampling with significant speedups. We combine the Tkatchenko-Scheffler van der Waals method (TS) and the many-body dispersion method (MBD) with third-order density functional tight-binding (DFTB3) via a charge population-based method. We find an overall good performance for the X23 benchmark database of molecular crystals, despite an underestimation of crystal volume that can be traced to the DFTB parametrization. We achieve accurate lattice energy predictions with DFT+MBD energetics on top of vdW-inclusive DFTB3 structures, resulting in a speedup of up to 3000 times compared with a full DFT treatment. This suggests that vdW-inclusive DFTB3 can serve as a viable structural prescreening tool in crystal structure prediction.