Ramos Chloe, Muehlbrad Jeremiah, Janesko Benjamin G
Department of Chemistry & Biochemistry, Texas Christian University, Fort Worth, Texas, USA.
J Comput Chem. 2021 Oct 15;42(27):1974-1981. doi: 10.1002/jcc.26728. Epub 2021 Aug 13.
We introduce the HF-R35-D3(BJ) functional combining full nonlocal exact (Hartree-Fock-like, HF) exchange, inexpensive rung-3.5 correlation constructed from nonlocal one-electron operators, and nonlocal D3 dispersion corrections. HF-R35-D3(BJ) is among the first full-exact-exchange functionals offering competitive accuracy for general main-group thermochemistry, kinetics, and noncovalent interactions. HF-R35-D3(BJ) gives weighted mean absolute deviation WTMAD-2 8.5 kcal/mol across the entire GMTKN55 dataset, outperforming most dispersion-corrected semilocal functionals and approaching the accuracy of dispersion-corrected global hybrids. This requires six fitted parameters, three each in the nonlocal correlation and dispersion corrections. Full nonlocal exchange appears to help give accurate binding energies and reasonable energy orderings for water hexamers. These results motivate continued exploration of inexpensive nonlocal correlation corrections to nonlocal exchange.
我们介绍了HF-R35-D3(BJ)泛函，它结合了完全非局部精确（类Hartree-Fock，HF）交换、由非局部单电子算符构建的低成本3.5级相关以及非局部D3色散校正。HF-R35-D3(BJ)是首批为一般主族热化学、动力学和非共价相互作用提供具有竞争力精度的完全精确交换泛函之一。HF-R35-D3(BJ)在整个GMTKN55数据集上给出的加权平均绝对偏差WTMAD-2为8.5 kcal/mol，优于大多数色散校正的半局部泛函，并且接近色散校正的全局杂化泛函的精度。这需要六个拟合参数，非局部相关和色散校正中各有三个。完全非局部交换似乎有助于给出准确的结合能和水六聚体合理的能量排序。这些结果促使人们继续探索对非局部交换进行低成本的非局部相关校正。
