Hoyer Chad E, Williams-Young David B, Huang Chen, Li Xiaosong
Department of Chemistry, University of Washington, Seattle, Washington 98195, USA.
Department of Scientific Computing, Materials Science and Engineering Program, and National High Magnetic Field Laboratory, Florida State University, Tallahassee, Florida 32306, USA.
J Chem Phys. 2019 May 7;150(17):174114. doi: 10.1063/1.5092628.
Spin-containing materials are important for spintronic applications. In this work, we present a computational framework to embed nonrelativistic, two-component calculations in a one-component environment. In this framework, both embedding scalar potential and magnetic field can be included to describe the interaction between quantum subsystems. In this current development, a generalized Kohn-Sham density functional theory electronic structure is embedded in unrestricted Kohn-Sham density functional theory. Two test systems are studied: a Li on a closed-shell He lattice and a Li on a He lattice containing a Li atom defect. The noncollinearity of Li is unaffected upon embedding in a closed-shell environment through the scalar potential embedding. However, the open-shell nature of the Li atom defect introduces an effective magnetic field that couples to the magnetic components of the generalized Kohn-Sham Hamiltonian. These results show that noncollinear quantum embedding in an open-shell collinear environment may modify the spin structure of the embedded system. The formalism developed herein may serve as a useful tool in the modeling of inhomogeneous magnetic fields in two-component calculations.
含自旋材料对于自旋电子学应用很重要。在这项工作中，我们提出了一个计算框架，用于在单组分环境中嵌入非相对论性的双组分计算。在此框架中，可以同时包含嵌入标量势和磁场来描述量子子系统之间的相互作用。在当前的发展中，广义的科恩 - 沙姆密度泛函理论电子结构被嵌入到无限制的科恩 - 沙姆密度泛函理论中。研究了两个测试系统：一个位于闭壳层氦晶格上的锂原子，以及一个位于含有锂原子缺陷的氦晶格上的锂原子。通过标量势嵌入将锂嵌入闭壳层环境时，锂的非共线性不受影响。然而，锂原子缺陷的开壳层性质引入了一个有效磁场，该磁场与广义科恩 - 沙姆哈密顿量的磁分量耦合。这些结果表明，在开壳层共线环境中的非共线量子嵌入可能会改变嵌入系统的自旋结构。本文所发展的形式体系可作为双组分计算中模拟非均匀磁场的有用工具。
