Sammanfattning
The gauge-including magnetically induced current (GIMIC) method for
calculating the components of the current-density tensor using gauge-including
atomic orbitals (GIAO) has been extended to treating open-shell molecules.
The applicability of the method is demonstrated by calculations of first-order
induced current densities on cyclobutadiene, Al3, and B3 at correlated
{\it ab initio} levels of theory. For comparison, current-density calculations
were also performed on the lowest closed-shell singlet state of cyclobutadiene
as well on the closed-shell Al3- and B3- anions. The ring-current
susceptibilities of the open-shell species are computed at the Hartree-Fock
self-consistent-field (HF-SCF), second-order M{\o}ller-Plesset perturbation
theory (MP2), and coupled-cluster singles and doubles (CCSD) levels, whereas
for the closed-shell systems also density functional theory (DFT) calculations
were employed. Explicit values for the current strengths caused by $\alpha$
and $\beta$ electrons as well as the difference, representing the spin
current, were obtained by numerical integration of the current-density
contributions passing a plane perpendicular to the molecular ring.
Comparisons of the present results to those recently obtained for the
lowest triplet state of biphenyl emphasize that electron correlation effects
must be considered for obtaining an accurate description of spin-current
densities.
Originalspråk | engelska |
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Tidskrift | Journal of Chemical Physics |
Volym | 134 |
Nummer | 5 |
Sidor (från-till) | 054123 |
Antal sidor | 12 |
ISSN | 0021-9606 |
DOI | |
Status | Publicerad - 2011 |
MoE-publikationstyp | A1 Tidskriftsartikel-refererad |
Vetenskapsgrenar
- 116 Kemi