Magnetic interactions in phenyl-bridged nitroxide diradicals: conformational effects by multireference and broken symmetry DFT approaches

J Phys Chem A. 2009 Dec 31;113(52):15150-5. doi: 10.1021/jp9053346.

Abstract

In the present paper we report the key results of a comprehensive computational study aimed at investigating the dependence of the singlet-triplet energy gap in phenyl-bridged bis-nitroxide diradicals, on the basis set and on soft structural parameters like torsion and pyramidalization. We have compared the BS-DFT technique with the post-Hartree-Fock DDCI2 multireference approach. With this latter method we have also studied the different role that sigma and pi core and virtual orbitals have in the resulting singlet-triplet energy gap.The results obtained represent one step forward in the definition of a protocol for an efficient and reliable computation of spin-spin coupling in diradical systems.

MeSH terms

  • Magnetics*
  • Models, Molecular
  • Molecular Conformation*
  • Nitrogen Oxides / chemistry*
  • Quantum Theory*
  • Reference Standards
  • Thermodynamics

Substances

  • Nitrogen Oxides
  • nitroxyl