Theoretical analysis of crystal field parameters and zero field splitting parameters for Mn2+ ions in tetramethylammonium tetrachlorozincate (TMATC-Zn)

A three-fold modeling approach of spectroscopic and magnetic properties of Mn2+-doped TMATC-Zn based on structural analysis performed. Semi-empirical superposition model calculations of crystal-field and zero-field splitting parameters carried out. Interstitial sites shown more plausible than substitutional sites for Mn2+, in agreement with EPR data. Comprehensive modeling of structural changes around 3dN centers shown useful for studying various materials, including Mn2+-based molecular nanomagnets. Range of applicability of our modeling approaches tested.