Magnetic-Field Density-Functional Theory (BDFT): Lessons from the Adiabatic Connection.
Magnetic-Field Density-Functional Theory (BDFT): Lessons from the Adiabatic Connection.
复制标题
磁场密度泛函理论 (BDFT)：绝热连接的经验教训。
DOI：
10.1021/acs.jctc.7b00295
复制
发表时间：
2017
影响因子：
5.5
通讯作者：
Reimann S
中科院分区：
文献类型：
--
作者：
Reimann S
我们在磁场密度泛函理论的背景下研究了磁场的影响，其中能量是电子密度ρ和磁场dB的泛函。我们表明，这种方法是一种有价值的替代电流密度泛函理论(CDFT)的方法，并可能为用密度泛函理论(DFT)研究许多磁现象提供一条可行的途径。在凸分析中鞍形函数及其凹凸母函数的四向对应的框架下，发展并阐明了BDFT和CDFT之间的关系。通过将能量分解为Kohn-Sham分量，我们证明了磁化率主要由与密度有关的能量分量决定。对于现有的密度泛函近似，这意味着，对于磁化能力，密度的改善将比在关联泛函中引入磁场相关性更有利。然而，一旦获得了良好的电荷密度，我们表明高精度可能只有通过考虑磁场相关性才能获得。我们证明了在不同场强下的绝热连接(AC)曲线彼此相似，只要每条曲线都是在该场强的平衡几何上计算的。相反，如果所有的交流曲线都是在无场系统的平衡几何上计算的，那么由于静态关联的重要性增加，曲线会随着场强的增加而发生强烈的变化。这也适用于密度泛函近似，对于密度泛函近似，我们证明了在零场强时遇到的主要误差已经存在，这表明密度泛函近似可以应用于强场中的系统，而不需要处理额外的静态关联。
We study the effects of magnetic fields in the context of magnetic field density-functional theory (BDFT), where the energy is a functional of the electron density ρ and the magnetic fieldB. We show that this approach is a worthwhile alternative to current-density functional theory (CDFT) and may provide a viable route to the study of many magnetic phenomena using density-functional theory (DFT). The relationship between BDFT and CDFT is developed and clarified within the framework of the four-way correspondence of saddle functions and their convex and concave parents in convex analysis. By decomposing the energy into its Kohn–Sham components, we demonstrate that the magnetizability is mainly determined by those energy components that are related to the density. For existing density functional approximations, this implies that, for the magnetizability, improvements of the density will be more beneficial than introducing a magnetic-field dependence in the correlation functional. However, once a good charge density is achieved, we show that high accuracy is likely only obtainable by including magnetic-field dependence. We demonstrate that adiabatic-connection (AC) curves at different field strengths resemble one another closely provided each curve is calculated at the equilibrium geometry of that field strength. In contrast, if all AC curves are calculated at the equilibrium geometry of the field-free system, then the curves change strongly with increasing field strength due to the increasing importance of static correlation. This holds also for density functional approximations, for which we demonstrate that the main error encountered in the presence of a field is already present at zero field strength, indicating that density-functional approximations may be applied to systems in strong fields, without the need to treat additional static correlation.
登录
查看更多内容
使用精确的耦合簇计算对旋转 g 张量和磁化率的密度泛函理论计算进行基准测试。
DOI：
10.1063/1.3242081
发表时间：
2009
期刊：
The Journal of chemical physics
影响因子：
--
作者：
O. Lutnaes;A. M. Teale;T. Helgaker;D. Tozer;K. Ruud;J. Gauss
通讯作者：
J. Gauss
密度泛函理论中的电流密度
影响因子：
2.9
作者：
E. Lieb;R. Schrader
通讯作者：
R. Schrader
影响因子：
2.9
作者：
Zhu, Wuming;Zhang, Liang;Trickey, S. B.
通讯作者：
Trickey, S. B.
影响因子：
2.9
作者：
Tellgren, Erik I.;Kvaal, Simen;Helgaker, Trygve
通讯作者：
Helgaker, Trygve
从完整构型相互作用密度计算绝热连接曲线：双电子系统。
影响因子：
4.4
作者：
A. M. Teale;S. Coriani;T. Helgaker
通讯作者：
T. Helgaker