First Principles Density-Based Embedding of Explicitly Correlated Systems

加州大学洛杉矶分校的艾米丽·卡特得到了理论和计算化学计划以及材料理论计划的支持，以开发凝聚态物质局部电子结构的第一性原理描述。方法的发展包括将一个小区域的电子结构的显式相关描述嵌入到周期性平板中，其电子结构由固态物理技术处理。将使用微扰理论等量子化学方法和密度泛函理论等本体方法。嵌入势将由涉及系统的总密度和嵌入区域的密度的项来构造。一个必然的项目涉及开发全球精确的动能密度泛函。测试应用包括一氧化碳和氧原子在过渡金属上的吸附。需要新的技术来可靠地预测凝聚相中反应和其他过程的准确能量。虽然密度泛函理论等第一性原理方法已经取得了非凡的成功，但它们的普遍适用性还没有得到证明。这项研究将对嵌入在块体材料中的局域区的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.