Ab initio molecular and solid state studies of Fe$^{II}$ spin cross-over system [Fe(btz)$_2$(NCS)$_2$

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Ab initio computations within the density functional theory are reported for the spin cross-over complex, [Fe(btz)$_{2}$(NCS)$_{2}$], where 3d$^6$ Fe$^{II}$ is characterized by High Spin (HS t$_{2g}^4$, e$_g^2$) and Low Spin (LS t$_{2g}^6$, e$_g^0$) states. Results of infra red and Raman spectra for the isolated molecule are complemented for the crystalline solid with a full account of the electronic band structure properties: the density of states assessing the crystal field effects and the chemical bonding assigning a specific role to the Fe-N interaction within the coordination sphere of Fe$^{II}$.

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