A reflection on modelling and examination of paramagnetic molecules for magnetic storage and molecular spintronics

Paramagnetic molecules featuring preferred orientation of their magnetic moments (magnetic anisotropy, single-molecule magnets, SMMs) are quite promising candidates for use in electronic devices like data storage and quantum computers (q-bits). In 2013, the authors published two papers on Fe^IIX₂ with pseudolinear cores (J. M. Zadrozny, M. Atanasov, A. M. Bryan, C.-Y. Lin, B. D. Rekken, P. P. Power, F. Neese, and J. R. Long, <i>Chem. Sci.</i>, 2013, <b>4</b>, 125-138, https://doi.org/10.1039/C2SC20801F and M. Atanasov, J. M. Zadrozny, J. R. Long and F. Neese, <i>Chem. Sci.</i>, 2013,<b>4</b>, 139-156, https://doi.org/10.1039/C2SC21394J). Combining computational tools with <i>ab initio</i> ligand field theory, design principles have been formulated to afford predictions of SMM prior to their later synthesis. These efforts resulted in a linear Co^IIC₂ SMM with magnetic anisotropy, the maximum possible for a 3d complex.