Surprisingly Good Performance of XYG3 Family Functionals Using a Scaled KS-MP3 Correlation,The Journal of Physical Chemistry Letters

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Surprisingly Good Performance of XYG3 Family Functionals Using a Scaled KS-MP3 Correlation
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2021-09-22 , DOI: 10.1021/acs.jpclett.1c02838
Golokesh Santra ₁ , Emmanouil Semidalas ₁ , Jan M L Martin ₁

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By adding a GLPT3 (third-order Görling-Levy perturbation theory, or KS-MP3) term E₃ to the XYG7 form for a double hybrid, we are able to bring down WTMAD2 (weighted total mean absolute deviation) for the very large and chemically diverse GMTKN55 benchmark to an unprecedented 1.17 kcal/mol, competitive with much costlier composite wave function ab initio approaches. Intriguingly, (a) the introduction of E₃ makes an empirical dispersion correction redundant; (b) generalized gradient approximation (GGA) or meta-GGA semilocal correlation functionals offer no advantage over the local density approximation (LDA) in this framework; (c) if a dispersion correction is retained, then simple Slater exchange leads to no significant loss in accuracy. It is possible to create a six-parameter functional with WTMAD2 = 1.42 that has no post-LDA density functional theory components and no dispersion correction in the final energy.

中文翻译：

使用缩放 KS-MP3 相关性的 XYG3 系列泛函性能出奇地好

通过将 GLPT3（三阶 Görling-Levy 微扰理论，或 KS-MP3）项E _{3 添加}到双混合的 XYG7 形式，我们能够降低 WTMAD2（加权总平均绝对偏差）化学多样化的 GMTKN55 基准达到前所未有的 1.17 kcal/mol，与更昂贵的复合波函数 ab initio 方法相竞争。有趣的是，(a) E ₃使经验色散校正变得多余；(b) 广义梯度近似 (GGA) 或元 GGA 半局部相关函数在该框架中没有提供优于局部密度近似 (LDA) 的优势；(c) 如果保留了色散校正，那么简单的 Slater 交换不会导致准确度的显着损失。可以创建一个 WTMAD2 = 1.42 的六参数泛函，它没有 LDA 后密度泛函理论分量，也没有最终能量的色散校正。

更新日期：2021-09-30

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