In:
The Journal of Chemical Physics, AIP Publishing, Vol. 151, No. 7 ( 2019-08-21)
Kurzfassung:
We revise formal and numerical aspects of collinear and noncollinear density functional theory (DFT) in the context of a two-component self-consistent treatment of spin-orbit coupling (SOC). While the extension of the standard one-component theory to a noncollinear magnetization is formally well-defined within the local density approximation, and therefore results in a numerically stable theory, this is not the case within the generalized gradient approximation (GGA). Previously reported formulations of noncollinear DFT based on GGA exchange-correlation potentials have several limitations: (i) they fail at reducing (either formally or numerically) to the proper collinear limit (i.e., when the magnetization is parallel or antiparallel to the z axis everywhere in space); (ii) they fail at ensuring a quantitative rotational invariance of the total energy and even a qualitative rotational invariance of the spatial distribution of the magnetization when a SOC operator is included in the Hamiltonian; (iii) they are numerically very unstable in regions of small magnetization. All of the above-mentioned problems are here shown (both formally and through test examples) to be solved by using instead a new formulation of noncollinear DFT for GGA functionals, which we call the “signed canonical” theory, as combined with an effective screening algorithm for unstable terms of the exchange-correlation potential in regions of small magnetization. All methods are implemented in the CRYSTAL program and tests are performed on simple molecules to compare the different formulations of noncollinear DFT. All three authors of the article agree to the retraction of the article effective April 16, 2021.
Materialart:
Online-Ressource
ISSN:
0021-9606
,
1089-7690
Sprache:
Englisch
Verlag:
AIP Publishing
Publikationsdatum:
2019
ZDB Id:
3113-6
ZDB Id:
1473050-9
Permalink
