Single-molecule Magnet Properties of Silole- and Stannole-ligated Erbium Cyclo-octatetraenyl Sandwich Complexes

硅杂环戊二烯和锡杂环戊二烯配位的铒环辛四烯夹心配合物的单分子磁性

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Abstract

The synthesis, structures and magnetic properties of an η(5)-silole complex and an η(5)-stannole complex of erbium are reported. The sandwich complex anions [(η(5)-Cp(Si))Er(η(8)-COT)](-) and [(η(5)-Cp(Sn))Er(η(8)-COT)](-), where Cp(Si) is [SiC(4)-2,5-(SiMe(3))(2)-3,4-Ph(2)](2-) (1(Si)), Cp(Sn) is [SnC(4)-2,5-(SiMe(3))(2)-3,4-Me(2)](2-) (1(Sn)) and COT=cyclo-octatetraenyl, were obtained as their [K(2.2.2-cryptand)](+) salts and found to be isostructural, with remarkably similar bond lengths and angles, differing only in the lengths of the Er-E interactions (E=Si, Sn). The parallels in the molecular structures of 1(Si) and 1(Sn) are reflected in their dynamic magnetic properties, which show single-molecule magnet behaviour in zero applied field, with effective energy barriers of 115±7 and 125±3 cm(-1), respectively, along with comparable magnetic relaxation times. Analysis of the two complexes using ab initio calculations reveals differences at a quantitative level, but overall similar electronic structures, with the thermally activated relaxation likely to proceed via the first-excited Kramers doublet. Comparing 1(Si) and 1(Sn) with the previously reported germanium analogue 1(Ge) reveals that swapping one heavier group 14 element for another in complexes of the type [(η(5)-Cp(E))Er(η(8)-COT)](-) has a minimal impact on the SMM behaviour.

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