Understanding the magnetization blocking mechanism in N23--radical-bridged dilanthanide single-molecule magnets

Herein, we report a theoretical investigation of the electronic structure and magnetic properties in [(Cp(2)(Me4H)Ln(THF))(2)(mu-N-2)](-) and [(Cp(2)(Me4H)Ln)(2)(mu-N-2)](-) (THF = tetrahydrofuran, Cp-Me4H = tetramethylcyclopentadienyl, Ln = Tb, Dy) complexes [as reported in Demir et al., Nat. Commun., 8, 1-9, 2144 (2017)]. By ab initio methods, their magnetic blocking behaviors are successfully characterized allowing elucidation of the origin of the two blocking barriers observed experimentally. In addition, a detailed analysis of exchange wave functions explains why the blocking barrier of the Tb complexes is roughly twice as large as that of the Dy analogues, a fact which appears to be a general trend exhibited in this family of compounds.

Automated summary

This theoretical investigation successfully characterized the electronic structure and magnetic properties of two complexes, explaining the origin of the observed blocking barriers experimentally and revealing a general trend where the blocking barrier of the Tb complexes is roughly twice as large as that of the Dy analogues in this family of compounds.