Ehlert Sebastian, Huniar Uwe, Ning Jinliang, Furness James W, Sun Jianwei, Kaplan Aaron D, Perdew John P, Brandenburg Jan Gerit
Mulliken Center for Theoretical Chemistry, University of Bonn, Beringstr. 4, 53115 Bonn, Germany.
Biovia, Dassault Systèmes Deutschland GmbH, Imbacher Weg 46, 51379 Leverkusen, Germany.
J Chem Phys. 2021 Feb 14;154(6):061101. doi: 10.1063/5.0041008.
We combine a regularized variant of the strongly constrained and appropriately normed semilocal density functional [J. Sun, A. Ruzsinszky, and J. P. Perdew, Phys. Rev. Lett. 115, 036402 (2015)] with the latest generation semi-classical London dispersion correction. The resulting density functional approximation rSCAN-D4 has the speed of generalized gradient approximations while approaching the accuracy of hybrid functionals for general chemical applications. We demonstrate its numerical robustness in real-life settings and benchmark molecular geometries, general main group and organo-metallic thermochemistry, and non-covalent interactions in supramolecular complexes and molecular crystals. Main group and transition metal bond lengths have errors of just 0.8%, which is competitive with hybrid functionals for main group molecules and outperforms them for transition metal complexes. The weighted mean absolute deviation (WTMAD2) on the large GMTKN55 database of chemical properties is exceptionally small at 7.5 kcal/mol. This also holds for metal organic reactions with an MAD of 3.3 kcal/mol. The versatile applicability to organic and metal-organic systems transfers to condensed systems, where lattice energies of molecular crystals are within the chemical accuracy (errors <1 kcal/mol).
我们将强约束且适当归一化的半局域密度泛函的正则化变体[J. 孙、A. 鲁辛斯基和J. P. 佩德韦，《物理评论快报》115, 036402 (2015)]与最新一代的半经典伦敦色散校正相结合。由此产生的密度泛函近似rSCAN-D4具有广义梯度近似的计算速度，同时在一般化学应用中接近杂化泛函的精度。我们在实际应用场景以及基准分子几何结构、一般主族和有机金属热化学，以及超分子复合物和分子晶体中的非共价相互作用方面展示了它的数值稳健性。主族和过渡金属键长的误差仅为0.8%，这与用于主族分子的杂化泛函相当，并且在过渡金属配合物方面优于它们。在大型化学性质GMTKN55数据库上的加权平均绝对偏差（WTMAD2）异常小，为7.5千卡/摩尔。对于金属有机反应，平均绝对偏差为3.3千卡/摩尔时也是如此。对有机和金属有机体系的广泛适用性也适用于凝聚体系，其中分子晶体的晶格能在化学精度范围内（误差<1千卡/摩尔）。
