论文标题
密度功能理论转化为单电子降低的密度基质功能理论，用于捕获静态相关
Density Functional Theory Transformed into a One-electron Reduced Density Matrix Functional Theory for the Capture of Static Correlation
论文作者
论文摘要
密度功能理论（DFT）是现代计算化学中最广泛采用的方法，无法准确描述强相关系统的电子结构。在这里，我们表明DFT可以正式，实际上可以转化为单电子降低密度 - 矩阵（1-RDM）功能理论，该理论可以解决DFT的局限性，同时与基于波函数的方法相比保留有利的计算缩放。除了在动能项中放宽对1-RDM的势力限制外，我们还为基于DFT的基于DFT的基于密度的交换 - 相关功能添加了一个基于二次的1-RDM项。我们通过DFT的$ O（r^{3}）$在DFT的计算缩放上实施的方法在化学结构和过程中的静态相关性（例如单线Biradicals和债券）等静态相关性的描述中，对传统DFT进行了实质性改进。
Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically transformed into a one-electron reduced-density-matrix (1-RDM) functional theory, which can address the limitations of DFT while retaining favorable computational scaling compared to wavefunction-based approaches. In addition to relaxing the idempotency restriction on the 1-RDM in the kinetic energy term, we add a quadratic 1-RDM-based term to DFT's density-based exchange-correlation functional. Our approach, which we implement by quadratic semidefinite programming at DFT's computational scaling of $O(r^{3})$, yields substantial improvements over traditional DFT in the description of static correlation in chemical structures and processes such as singlet biradicals and bond dissociations.
