论文标题

正则扫描功能与扫描功能的比较,具有和不进行自我交流的功能

Comparison of regularized SCAN functional with SCAN functional with and without self-interaction for a wide-array of properties

论文作者

Yamamoto, Yoh, Salcedo, Alan, Diaz, Carlos M., Alam, Md Shamsul, Baruah, Tunna, Zope, Rajendra R.

论文摘要

受到严格限制和适当的规范(SCAN)功能是一种非经验的元元元素梯度近似(meta-GGGA)功能,它满足了元gga功能易值的所有已知约束,但它也表现出对数值网格的极大敏感性。当在Perdew-Zunger(PZ)自我相互作用校正(SIC)中使用时,它的数值复杂性会放大,该校正(SIC)需要使用轨道密度来评估能量和电势,而轨道密度却比自旋密度差得多。扫描功能(RSCAN)的最新正规化简化了扫描的数值复杂性,而牺牲了某些确切的约束。为了对RSCAN的性能有很好的了解以及在慢慢变化的限制下丢失精确约束的影响,我们将其性能与振动频率,水簇的振动频率,红外和拉曼强度的扫描进行了比较分子。同样,我们通过研究原子总能量,电离电位和电子亲和力,分子雾化能,屏障高度以及解离和反应能来检查SIC-RSCAN的性能。我们发现,RSCAN需要的密度要少得多,并给出非常相似的结果,因为扫描所有检查的属性,但在RSCAN中的雾化能有所更糟。另一方面,对于这项工作中研究的几乎所有属性,SIC-RSCAN比SIC-SCAN的性能比SIC-SCAN略有。

The Strongly Constrained and Appropriately Normed (SCAN) functional is a non-empirical meta-generalized-gradient approximation (meta-GGA) functional that satisfies all the known constraints that a meta-GGA functional can, but it also exhibits a great degree of sensitivity to numerical grids. Its numerical complexities are amplified when used in Perdew-Zunger (PZ) self-interaction correction (SIC) which requires evaluating energies and potentials using orbital densities that vary far more rapidly than spin densities. Recent regularization of the SCAN functional (rSCAN) simplifies numerical complexities of SCAN at the expense of violation of some exact constraints. To develop a good understanding of the performance of rSCAN and the effect of loss of an exact constraint at the limit of slowly varying density, we have compared its performance against SCAN for vibrational frequencies, infra-red and Raman intensities of water clusters, electric dipole moments, spin magnetic moments of a few molecular magnets, weak interaction energies of dimers, barrier heights of reactions, and atomization energies for benchmark sets of molecules. Likewise, we examined the performance of SIC-rSCAN using the PZ-SIC method by studying atomic total energies, ionization potentials and electron affinities, molecular atomization energies, barrier heights, and dissociation and reaction energies. We find that rSCAN requires a much less dense numerical grid and gives very similar results as SCAN for all properties examined with the exception of atomization energies which are somewhat worse in rSCAN. On the other hand, SIC-rSCAN gives marginally better performance than SIC-SCAN for almost all properties studied in this work.

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