Theory and Simulation of Materials (THEOS), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland.
School of Natural and Environmental Sciences, Newcastle University, Newcastle upon Tyne NE1 7RU, United Kingdom.
J Chem Theory Comput. 2020 Aug 11;16(8):4899-4911. doi: 10.1021/acs.jctc.0c00162. Epub 2020 Jun 9.
We introduce the unification of dynamical mean field theory (DMFT) and linear-scaling density functional theory (DFT), as recently implemented in ONETEP, a linear-scaling DFT package, and TOSCAM, a DMFT toolbox. This code can account for strongly correlated electronic behavior while simultaneously including the effects of the environment, making it ideally suited for studying complex and heterogeneous systems that contain transition metals and lanthanides, such as metalloproteins. We systematically introduce the necessary formalism, which must account for the nonorthogonal basis set used by ONETEP. In order to demonstrate the capabilities of this code, we apply it to carbon monoxide ligated iron porphyrin and explore the distinctly quantum-mechanical character of the iron 3d electrons during the process of photodissociation.
我们介绍了动力学平均场理论 (DMFT) 和线性标度密度泛函理论 (DFT) 的统一，这是最近在 ONETEP（一种线性标度 DFT 包）和 TOSCAM（一种 DMFT 工具箱）中实现的。该代码可以解释强相关电子行为，同时包括环境的影响，因此非常适合研究包含过渡金属和镧系元素的复杂和异质系统，例如金属蛋白。我们系统地介绍了必要的形式主义，它必须考虑到 ONETEP 使用的非正交基集。为了展示该代码的功能，我们将其应用于一氧化碳配位的铁卟啉，并研究了光解过程中铁 3d 电子的明显量子力学特征。
