论文标题

研究使用三种自我交互校正方法的磁性交换耦合常数密度功能计算中的自我交流误差的研究

Study of Self-Interaction Errors in Density Functional Calculations of Magnetic Exchange Coupling Constants Using Three Self-Interaction Correction Methods

论文作者

Mishra, Prakash, Yamamoto, Yoh, Chang, Po-Hao, Nguyen, Duyen B., Peralta, Juan E., Baruah, Tunna, Zope, Rajendra R.

论文摘要

我们研究了自我交互误差(SIE)在评估磁交换耦合常数中的作用。特别是,我们分析了三个{\ em非经验}密度函数近似值(DFAS)的缩小自身交互 - 校正(SIC)的效果,即局部自旋密度近似,Perdew-Burke-ernzerhof广义梯度近似,最近的scan scan scan家族元元素型元元素。为此,我们采用了三种单电子SIC方法:Perdew-Zunger [Perdew,J。P。; Zunger,A。\ textit {phys。 Rev. b},{\ bf 1981},\ textit {23},5048] sic,OrbitalWise缩放的SIC方法[Vydrov,O。A. \ textit {et al。},\ textit {j。化学物理。} {\ bf 2006,} \ textIt {124},094108]和最近的{local}缩放方法[Zope,R。R. R. R. \ textit {et al。},\ textit {j。化学Phys。} {\ bf 2019},\ textit {151},214108]。我们使用自旋投影和非投影方法计算磁交换偶联常数,用于由双核和多核H-模型,有机自由基分子和氯化酸盐组成的分子集,并将这些结果与准确的理论和实验进行比较。我们的结果表明,对于主要由单个电子区域组成的系统,PZSIC的性能良好,但对于更复杂的有机系统和氯化酸盐,PZSIC的过度正确趋势与这项工作中使用的DFA相结合,在这种情况下更为明显,在这种情况下,与动力学能量密度比率相比,PZSIC的性能更好。根据SIC校正对密度和总能量的分析表明,要改善磁交换耦合的预测,需要密度和能量校正。

We examine the role of self-interaction errors (SIE) removal on the evaluation of magnetic exchange coupling constants. In particular we analyze the effect of scaling down the self-interaction-correction (SIC) for three {\em non-empirical} density functional approximations (DFAs) namely, the local spin density approximation, the Perdew-Burke-Ernzerhof generalized gradient approximation, and recent SCAN family of meta-GGA functionals. To this end, we employ three one-electron SIC methods: Perdew-Zunger [Perdew, J. P.; Zunger, A. \textit{Phys. Rev. B}, {\bf 1981}, \textit{23}, 5048] SIC, the orbitalwise scaled SIC method [Vydrov, O. A. \textit{et al.}, \textit{J. Chem. Phys.} {\bf 2006,} \textit{124}, 094108], and the recent {local} scaling method [Zope, R. R. \textit{et al.}, \textit{J. Chem. Phys.} {\bf 2019}, \textit{151}, 214108]. We compute the magnetic exchange coupling constants using the spin projection and non projection approaches for sets of molecules composed of dinuclear and polynuclear H--He models, organic radical molecules, and chlorocuprate, and compare these results against accurate theories and experiment. Our results show that for the systems that mainly consist of single electron regions, PZSIC performs well but for more complex organic systems and the chlorcuprates, an overcorrecting tendency of PZSIC combined with the DFAs utilized in this work is more pronounced, and in such cases LSIC with kinetic energy density ratio performs better than PZSIC. Analysis of the results in terms of SIC corrections to the density and to the total energy shows that both density and energy correction are required to obtain an improved prediction of magnetic exchange couplings.

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