Insensitivity of Magnetic Coupling to Ligand Substitution in a Series of Tetraoxolene Radical-Bridged Fe2 Complexes
Abstract
The elucidation of magnetostructural correlations between bridging ligand substitution and strength of magnetic coupling is essential to the development of high-temperature molecule-based magnetic materials. Toward this end, we report the series of tetraoxolene-bridged FeII2 complexes [(Me3TPyA)2Fe2(RL)]n+ (Me3TPyA = tris(6-methyl-2-pyridylmethyl)amine; n = 2: OMeLH2 = 3,6-dimethoxy-2,5-dihydroxo-1,4-benzoquinone, ClLH2 = 3,6-dichloro-2,5-dihydroxo-1,4-benzoquinone, Na2[NO2L] = sodium 3,6-dinitro-2,5-dihydroxo-1,4-benzoquinone; n = 4: SMe2L = 3,6-bis(dimethylsulfonium)-2,5-dihydroxo-1,4-benzoquinone diylide) and their one-electron-reduced analogues. Furthermore, variable-temperature dc magnetic susceptibility data reveal the presence of weak ferromagnetic superexchange between FeII centers in the oxidized species, with exchange constants of J = +1.2(2) (R = OMe, Cl) and +0.3(1) (R = NO2, SMe2) cm–1. In contrast, X-ray diffraction, cyclic voltammetry, and Mössbauer spectroscopy establish a ligand-centered radical in the reduced complexes. Magnetic measurements for the radical-bridged species reveal the presence of strong antiferromagnetic metal–radical coupling, with J = -57(10), -60(7), -58(6), and -65(8) cm–1 for R = OMe, Cl, NO2, and SMe2, respectively. The minimal effects of substituents in the 3- and 6-positions of RLx–• on the magnetic coupling strength is understood through electronic structure calculations, which show negligible spin density on the substituents and associated C atoms of the ring. Finally, the radical-bridged complexes are single-molecule magnets, with relaxation barriers of Ueffmore »
- Authors:
-
[1];
[2];
[3]
- Northwestern Univ., Evanston, IL (United States)
- Max-Planck-Inst. für Chemische Energiekonversion, Mülheim an der Ruhr (Germany)
- Northwestern Univ., Evanston, IL (United States); Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF)
- OSTI Identifier:
- 1803720
- Grant/Contract Number:
- SC0019356; NNCI-1542205
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Inorganic Chemistry
- Additional Journal Information:
- Journal Volume: 59; Journal Issue: 7; Journal ID: ISSN 0020-1669
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Redox reactions; Ligands; Substituents; Magnetic properties; Quantum mechanics
Citation Formats
Thorarinsdottir, Agnes E., Bjornsson, Ragnar, and Harris, T. David. Insensitivity of Magnetic Coupling to Ligand Substitution in a Series of Tetraoxolene Radical-Bridged Fe2 Complexes. United States: N. p., 2020.
Web. doi:10.1021/acs.inorgchem.9b03736.
Thorarinsdottir, Agnes E., Bjornsson, Ragnar, & Harris, T. David. Insensitivity of Magnetic Coupling to Ligand Substitution in a Series of Tetraoxolene Radical-Bridged Fe2 Complexes. United States. https://doi.org/10.1021/acs.inorgchem.9b03736
Thorarinsdottir, Agnes E., Bjornsson, Ragnar, and Harris, T. David. Fri .
"Insensitivity of Magnetic Coupling to Ligand Substitution in a Series of Tetraoxolene Radical-Bridged Fe2 Complexes". United States. https://doi.org/10.1021/acs.inorgchem.9b03736. https://www.osti.gov/servlets/purl/1803720.
@article{osti_1803720,
title = {Insensitivity of Magnetic Coupling to Ligand Substitution in a Series of Tetraoxolene Radical-Bridged Fe2 Complexes},
author = {Thorarinsdottir, Agnes E. and Bjornsson, Ragnar and Harris, T. David},
abstractNote = {The elucidation of magnetostructural correlations between bridging ligand substitution and strength of magnetic coupling is essential to the development of high-temperature molecule-based magnetic materials. Toward this end, we report the series of tetraoxolene-bridged FeII2 complexes [(Me3TPyA)2Fe2(RL)]n+ (Me3TPyA = tris(6-methyl-2-pyridylmethyl)amine; n = 2: OMeLH2 = 3,6-dimethoxy-2,5-dihydroxo-1,4-benzoquinone, ClLH2 = 3,6-dichloro-2,5-dihydroxo-1,4-benzoquinone, Na2[NO2L] = sodium 3,6-dinitro-2,5-dihydroxo-1,4-benzoquinone; n = 4: SMe2L = 3,6-bis(dimethylsulfonium)-2,5-dihydroxo-1,4-benzoquinone diylide) and their one-electron-reduced analogues. Furthermore, variable-temperature dc magnetic susceptibility data reveal the presence of weak ferromagnetic superexchange between FeII centers in the oxidized species, with exchange constants of J = +1.2(2) (R = OMe, Cl) and +0.3(1) (R = NO2, SMe2) cm–1. In contrast, X-ray diffraction, cyclic voltammetry, and Mössbauer spectroscopy establish a ligand-centered radical in the reduced complexes. Magnetic measurements for the radical-bridged species reveal the presence of strong antiferromagnetic metal–radical coupling, with J = -57(10), -60(7), -58(6), and -65(8) cm–1 for R = OMe, Cl, NO2, and SMe2, respectively. The minimal effects of substituents in the 3- and 6-positions of RLx–• on the magnetic coupling strength is understood through electronic structure calculations, which show negligible spin density on the substituents and associated C atoms of the ring. Finally, the radical-bridged complexes are single-molecule magnets, with relaxation barriers of Ueff = 50(1), 41(1), 38(1), and 33(1) cm–1 for R = OMe, Cl, NO2, and SMe2, respectively. Taken together, these results provide the first examination of how bridging ligand substitution influences magnetic coupling in semiquinoid-bridged compounds, and they establish design criteria for the synthesis of semiquinoid-based molecules and materials.},
doi = {10.1021/acs.inorgchem.9b03736},
journal = {Inorganic Chemistry},
number = 7,
volume = 59,
place = {United States},
year = {Fri Mar 20 00:00:00 EDT 2020},
month = {Fri Mar 20 00:00:00 EDT 2020}
}
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