Observation of internal electron transfer in bulky allyl ytterbium complexes with substituted terpyridine ligands |
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Authors: | White Rosemary E Carlson Christin N Veauthier Jacqueline M Simpson Cheslan K Thompson J D Scott Brian L Hanusa Timothy P John Kevin D |
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Institution: | Department of Chemistry, Vanderbilt University, Nashville, TN 37235, USA. |
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Abstract: | A series of new bulky allyl terpyridyl-ytterbium complexes have been synthesized to determine the effect of allyl ligands on the internal charge-transfer process that exists in these materials. Compared to the pentamethylcyclopentadienyl-ytterbocene compound Cp*2Yb(tpyCN) (nu(C(triple bond)N) = 2172 cm(-1)), the symmetrically substituted allyl complex 1,3-(SiMe3)2C3H3]2Yb(tpyCN) possesses a markedly lowered C(triple bond)N frequency of 2130 cm(-1). Furthermore, the electronic nature of these bulky allyl complexes can be tuned, as demonstrated by the C(triple bond)N frequency of the asymmetric derivatives 1-(SiMe3)C3H4]2Yb(tpyCN) and 1-(SiPh3)-3-(SiMe3)C3H3]2Yb(tpyCN) (2171 and 2164 cm(-1), respectively). The differences in these frequencies can be attributed to differences in the ligands' steric and electronic character. Single-crystal X-ray characterization of 1,3-(SiMe3)2C3H3]2Yb(tpy) reveals that the allyl moiety possesses shorter Yb-C and Yb-N bond distances than the Cp* analogue. The magnetic susceptibility data for 1,3-(SiMe3)2C3H3]2Yb(tpy) departs dramatically from the Curie law, with a room-temperature magnetic moment of 2.95 mu(B). |
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