Magnetic exchange couplings from constrained density functional theory: an efficient approach utilizing analytic derivatives.
Magnetic exchange couplings from constrained density functional theory: an efficient approach utilizing analytic derivatives.
复制标题
约束密度泛函理论的磁交换耦合：利用解析导数的有效方法。
DOI：
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发表时间：
2011
影响因子：
4.4
通讯作者：
J. Peralta
中科院分区：
文献类型：
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作者：
J. Phillips;J. Peralta
我们介绍了一种基于Rudra，Wu和货车Voorhis [J. Chem. Phys. 124，024103（2006）]的约束密度泛函理论（C-DFT）方法评估磁交换耦合的方法。我们的方法与C-DFT具有相同的物理原理，但利用了电子能量在感兴趣的范围内相对于约束二次和双线性变化的事实。这使我们能够使用耦合微扰Kohn-Sham自旋密度泛函理论来近似地确定不同自旋构型的能量的校正，并先验地构建由约束自旋密度泛函理论获得的相关能量景观。我们评估这种方法在一组双核过渡金属配合物，并表明，它再现非常密切的C-DFT的结果。这证明了这种方法作为研究许多其他分子现象的潜在工具的概念验证。此外，路线，以改善这种方法的局限性进行了讨论。
We introduce a method for evaluating magnetic exchange couplings based on the constrained density functional theory (C-DFT) approach of Rudra, Wu, and Van Voorhis [J. Chem. Phys. 124, 024103 (2006)]. Our method shares the same physical principles as C-DFT but makes use of the fact that the electronic energy changes quadratically and bilinearly with respect to the constraints in the range of interest. This allows us to use coupled perturbed Kohn-Sham spin density functional theory to determine approximately the corrections to the energy of the different spin configurations and construct a priori the relevant energy-landscapes obtained by constrained spin density functional theory. We assess this methodology in a set of binuclear transition-metal complexes and show that it reproduces very closely the results of C-DFT. This demonstrates a proof-of-concept for this method as a potential tool for studying a number of other molecular phenomena. Additionally, routes to improving upon the limitations of this method are discussed.