Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 133, Issue 40, Pages 15806-15809Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja203845x
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- University of Ottawa
- CCRI
- CFI
- FFCR
- NSERC
- ERA
- U.S. DOE Office of Energy Efficiency and Renewable Energy
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Two mononuclear high-spin Fe-II complexes with trigonal planar ([Fe-II(N(TMS)(2))(2)(PCy3)] (1) and distorted tetrahedral ([Fe-II(N(TMS)(2))(2)(depe)] (2) geometries are reported (TMS = SiMe3, Cy = cyclohexyl, depe = 1,2-bis(diethylphosphino)ethane). The magnetic properties of 1 and 2 reveal the profound effect of out-of-state spin-orbit coupling (SOC) on slow magnetic relaxation. Complex 1 exhibits slow relaxation of the magnetization under an applied optimal dc field of 600 Oe due to the presence of low-lying electronic excited states that mix with the ground electronic state. This mixing re-introduces orbital angular momentum into the electronic ground state via SOC, and 1 thus behaves as a field-induced single. molecule magnet. In complex 2, the lowest-energy excited states have higher energy due to the ligand field of the distorted tetrahedral geometry. This higher energy gap minimizes out-of-state SOC mixing and zero-field splitting, thus precluding slow relaxation of the magnetization for 2.
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