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Rhodamine Salicylaldehyde Hydrazone Dy(III) Complexes: Fluorescence and Magnetism.
Inorganic Chemistry 2018 April 3
Three new dysprosium(III) complexes [Dy2 (HL1 -o)2 (L1 )(NO3 )3 ][Dy(NO3 )5 ]·1.5ACE·0.5Et2 O (1), [Dy(L1 )3 ]·2.5MeOH·MeCN (2), and [Dy(L2 )3 ]·MeOH·MeCN (3) (HL1 = rhodamine B salicylaldehyde hydrazine, HL2 = rhodamine B 3-methylsalicylaldehyde hydrazine) were synthesized and characterized. Purple complex 1 contains two ring-open ligands HL1 -o and shows fluorescence of the rhodamine amide moiety, whereas yellow complexes 2 and 3 are comprised of ring-close ligands (L1/2 )- and display fluorescence of the salicylaldehyde Schiff base part. For 2 and 3, Dy(III) ions are nine coordinated by the six oxygen and three nitrogen atoms of three chelate (L1/2 )- ligands, but the arrangements of the three ligands are different owing to the methyl substituent on HL2 . There are three short predominant Dy-Ophenoxy bonds in 2 and 3. The largest Ophenoxy -Dy-Ophenoxy angle is 148.64(17)° for 2 and 89.63(13)° for 3. Magnetic studies reveal that complex 2 is a field-induced single-molecule magnet ( Ueff = 104.2 K under a dc magnetic field of 2000 Oe), and 3 exhibits only a magnetic relaxation behavior owing to the quantum tunneling of magnetization (QTM). Furthermore, ab initio calculations illustrate that the disposition of predominant Dy-Ophenoxy bonds affects the magnetic anisotropy of the Dy(III) ions and relaxation processes of complexes 2 and 3.
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