论文标题
小分子与石墨烯样薄片之间的分散相互作用的计算研究
Computational investigations of dispersion interactions between small molecules and graphene-like flakes
论文作者
论文摘要
在这项工作中，我们研究了在选择原子，分子和分子表面系统中的分散相互作用，将高级相关方法与经验校正的密度功能理论（DFT）进行了比较。我们评估了通常用于基于表面计算的功能的功能，并进行了有或没有Grimme校正的功能。我们发现，校正的包含对于获得有意义的结果至关重要，但是否则几乎没有区分功能。我们还使用新型的绝对局部局部分子轨道的方法，提出了\ ce {h2}和\ ce {no2}与大碳表面相互作用的耦合群集质量相互作用曲线。这些计算表明，在研究色散时，经验校正的DFT的问题随着系统大小的增加而似乎复杂化，这对分子表面相互作用的未来计算研究具有重要意义。
In this work, we investigate dispersion interactions in a selection of atomic, molecular, and molecule-surface systems, comparing high-level correlated methods with empirically-corrected density functional theory (DFT). We assess the efficacy of functionals commonly used for surface-based calculations, with and without the D3 correction of Grimme. We find that the inclusion of the correction is essential to get meaningful results, but there is otherwise little to distinguish between the functionals. We also present coupled-cluster quality interaction curves for \ce{H2} and \ce{NO2} interacting with large carbon flakes, acting as models for graphene surfaces, using novel absolutely localised molecular orbital based methods. These calculations demonstrate that the problems with empirically-corrected DFT when investigating dispersion appear to compound as the system size increases, with important implications for future computational studies of molecule-surface interactions.
