DFT Computational Rationalization of an Unusual Spin Ground State in an Mn12 Single‐Molecule Magnet with a Low‐Symmetry Loop Structure

Loopy about magnetism: The use of N-methyldiethanolamine (mdaH2) leads to new Mn12 and Mn4 single-molecule magnets (SMMs) with S=7 and S=9 ground-state spins, respectively. The Mn12 species (see structure: MnIII green, MnII orange, O red, N blue, C gray) is a rare example of an SMM with a loop structure. Its unusual S=7 ground state for an MnIII6MnII6 species is rationalized by DFT calculations.