Title :

Spin-orbit coupling from a two-component self-consistent approach. I. Generalized Hartree-Fock theory

Author(s) :

Desmarais, Jacques [Auteur]
Università degli studi di Torino = University of Turin [UNITO]
Institut des sciences analytiques et de physico-chimie pour l'environnement et les materiaux [IPREM]
Flament, Jean-Pierre [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Erba, Alessandro [Auteur]
Nanostructured Interfaces and Surfaces Centre [NIS ]

Journal title :

The Journal of Chemical Physics

Publisher :

American Institute of Physics

Publication date :

2019-08-21

ISSN :

0021-9606

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

Formal and computational aspects are discussed for a self-consistent treatment of spin-orbit coupling within the two-component generalization of the Hartree-Fock theory. A molecular implementation into the CRYSTAL program ...
Show more >Formal and computational aspects are discussed for a self-consistent treatment of spin-orbit coupling within the two-component generalization of the Hartree-Fock theory. A molecular implementation into the CRYSTAL program is illustrated, where the standard one-component code (typical of Hartree-Fock and Kohn-Sham spin-unrestricted methodologies) is extended to work in terms of two-component spinors. When passing from a one- to a two-component description, the Fock and density matrices become complex. Furthermore, apart from the αα and ββ diagonal spin blocks, one has also to deal with the αβ and βα off-diagonal spin blocks. These latter blocks require special care as, for open-shell electronic configurations, certain constraints of the one-component code have to be relaxed. This formalism intrinsically allows us to treat local magnetic torque as well as noncollinear magnetization and orbital current-density. An original scheme to impose a specified noncollinear magnetization on each atomic center as a starting guess to the self-consistent procedure is presented. This approach turns out to be essential to surpass local minima in the rugged energy landscape and allows possible convergence to the ground-state solution in all of the discussed test cases.Show less >

Language :

Anglais

Popular science :

Non

Collections :

• Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL

Submission date :

2024-09-17T02:39:42Z