论文标题

密度函数基于DFT强相互作用极限的数学结构

Density Functionals based on the mathematical structure of the strong-interaction limit of DFT

论文作者

Vuckovic, Stefan, Gerolin, Augusto, Daas, Timothy J., Bahmann, Hilke, Friesecke, Gero, Gori-Giorgi, Paola

论文摘要

原则上,Kohn-Sham密度功能理论(计算化学的主力)必须依靠近似值来进行交换 - 相关功能。尽管取得了惊人的成功,但当电子 - 电子相关性的影响起着重要作用时,当今的近似值仍然很困难。电子库仑排斥完全主导交换相关功能的极限提供了一个定义明确的数学框架,可为能够处理强相关性的新近似值提供见解。特别是,由于其重新制定为最佳运输问题,该限制的数学结构现在已经建立了良好,这表明使用非常不同的成分(或特征)相对于当前近似值中使用的成分(或特征)。我们专注于使用这些新成分来建立计算化学的近似值,并强调未来有希望的方向。

While in principle exact, Kohn-Sham density functional theory -- the workhorse of computational chemistry -- must rely on approximations for the exchange-correlation functional. Despite staggering successes, present-day approximations still struggle when the effects of electron-electron correlation play a prominent role. The limit in which the electronic Coulomb repulsion completely dominates the exchange-correlation functional offers a well-defined mathematical framework that provides insight for new approximations able to deal with strong correlation. In particular, the mathematical structure of this limit, which is now well-established thanks to its reformulation as an optimal transport problem, points to the use of very different ingredients (or features) with respect to the traditional ones used in present approximations. We focus on strategies to use these new ingredients to build approximations for computational chemistry and highlight future promising directions.

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