Evaluating the energy difference between different spin states including, in particular, the high-spin (HS) and low-spin (LS) spilitting ?EH-L in the spin-crossover (SCO) compounds and the Heisenberg exchange coupling constant J in polynuclear complexes, is still a great challenge in theoretical chemistry. In this work, we first establish the performance of the density functional theory plus the Hubbard U (DFT+U) approach to describe intra- and inter-atomic spin interactions using a series of archetypal 3d transition metal complexes as model systems [1]. We then use the DFT+U approach to investigate the mechanism underlying the magnetic interactions in a set of prototypical CuII-GdIII 3d-4f systems. By combining DFT+U with the van der Waals functional for non-covalent interactions, we also investigate the influence of crystal packing on the spin-transition behavior in several FeII spin-crossover molecular crystal materials. [1] Zhang, Y.; Jiang, H. J. Chem. Theory Comput. 20 11 , 7, 2795.

Intra- and inter-atomic magnetic interactions in molecular magnetism: The role of on-site Coulomb interaction and crystal packing

243rd National Meeting (2012)

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