First Principles Density-Based Embedding of Explicitly Correlated Systems

加州大学洛杉矶分校的Emily Carter得到了理论与计算化学项目和材料理论项目的支持，以发展凝聚态物质局部电子结构的第一性原理描述。方法开发包括将小区域电子结构的显式相关描述嵌入到通过固态物理技术处理电子结构的周期板中。量子化学方法，如微扰理论和体方法，如密度泛函理论将被采用。嵌入势将由涉及系统总密度和嵌入区域密度的项来构造。一个必然的项目涉及开发全局精确的动能密度泛函。测试应用包括一氧化碳和氧原子对过渡金属的吸附。需要新的技术来准确可靠地预测反应和其他凝聚相过程的能量学。虽然密度泛函理论等第一性原理方法取得了非凡的成功，但它们的普遍适用性尚未得到证实。本研究将对块状材料中局部区域能量学的密度泛函理论进行系统的改进。

Emily Carter of UCLA is supported by the Theoretical and Computational Chemistry Program and the Materials Theory Program to develop first-principles descriptions of the local electronic structure of condensed matter. Method development includes embedding an explicitly correlated description of the electronic structure of a small region into a periodic slab whose electronic structure is treated by solid-state physics techniques. Quantum chemical methods such as perturbation theory and bulk methods such as density functional theory will be employed. The embedding potential will be constructed from terms involving the total density of the system and the density of the embedded region. A corollary project involves the development of globally accurate kinetic energy density functionals. Test applications include carbon monoxide and oxygen atom adsorption on transition metals.New techniques are required to reliably predict accurate energetics of reactions and other processes in the condensed phase. While some first-principles methods such as density functional theory have had extraordinary success, their general applicability has not been proven. This research will pursue a systematic improvement to density functional theory for the energetics of a localized region embedded in a bulk material.