NDLI: Unsymmetrical diimine complexes of iron(II) and manganese(II): synthesis, structure and photoluminescence of an isomer

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Unsymmetrical diimine complexes of iron(II) and manganese(II): synthesis, structure and photoluminescence of an isomer

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Roy, Amit Saha Ghosh, Prasanta Biswas, Manas Kumar Weyhermüller, Thomas
Description	Author Affiliation: Roy AS ( Department of Chemistry, R. K. Mission Residential College, Narendrapur, Kolkata-103, India.)
Abstract	Two bis(unsymmetrical diimine ) complexes of $(L_{NO2}^{ϕ1})(L_{NO2}^{ϕ2})M^{II}Cl_{2}$ family with M = Fe and Mn, are reported $(L_{NO2}^{ϕ}$ = ( E)-3-nitro- N-(pyridine-2-ylmethylene)aniline ; ϕ = dihedral angle between the diimine unit including pyridine ring and the phenyl ring planes). Pure $tcc-(L_{NO2}^{33.6})(L_{NO2}^{79.3})Fe^{II}Cl_{2}·0.5H_{2}O$ (1) and $tcc-(L_{NO2}^{32.0})(L_{NO2}^{79.4})Mn^{II}Cl_{2}·0.5H_{2}O$ (2) isomers have been successfully isolated in high yields and characterized by elemental analyses, variable temperature magnetic susceptibility measurements, IR , mass, UV-vis and Mössbauer spectra including the single-crystal X-ray structure determinations that identified strong intermolecular non-bonding interactions in lattice (tcc refers to trans–cis–cis positions with respect to pyridine N-imine N–Cl donors). Geometries optimizations of all possible tcc, ttt, ctc, ccc and cct isomers of iron at the B3LYP/DFT level in gas-phase have shown that the tcc-isomer incorporating two non-equivalent ligands as in $(L_{NO2}^{42})(L_{NO2}^{61})Fe^{II}Cl_{2},$ 1 (g), is stabilized by 6–20 kJ $mol^{−1}$ compared to other isomers where two ligands are equivalent. The frozen methanol glasses of 1 and 2 are luminescent at 77 K (1: $λ_{ext}$ = 370, $λ_{em}$ = 521 nm, $χ^{2}$ = 1.3, $τ_{avg}$ = 0.57 ns; 2: $λ_{ext}$ = 368, $λ_{em}$ = 524 nm, $χ^{2}$ = 1.1, $τ_{avg}$ = 0.90 ns). The DFT calculations have identified four closely spaced localized $π^{*}$ orbitals comprising of two non-equivalent ligands as UPMOs. The features contrast the tcc-isomer of $(L^{ϕ})_{2}Fe^{II}Cl_{2}$ (3), congener of 1 without $–NO_{2}$ substitution and non-emissive $(bpy)_{2}Fe^{II}Cl_{2}$ (4) where two ligands are equivalent. TD-DFT calculations have assigned intra- ligand (IL) and ligand to ligand charge transfer (LLCT) dominated excited states as the origin of luminescence of 1 and 2.
ISSN	14779226
Issue Number	1
Volume Number	40
e-ISSN	13645447
Journal	Dalton Trans.
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2011-01-07
Publisher Place	Great Britain (UK)
Access Restriction	Subscribed
Subject Keyword	Ferrous Compounds Chemistry Imines Manganese Crystallography, X-Ray Chemical Synthesis Luminescence Models, Molecular Quantum Theory Spectrophotometry, Ultraviolet Spectroscopy, Fourier Transform Infrared Spectroscopy, Mossbauer Stereoisomerism Journal Article Research Support, Non-U.S. Gov't
Content Type	Text
Resource Type	Article
Subject	Inorganic Chemistry

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