Slow magnetization dynamics in Co(ii)/Co(iii) triethanolamine/pivalate complexes
We report the synthesis, structural characterization and a combined computational and experimental study of the magnetic properties of two pivalate cobalt complexes, a mononuclear Co(ii) one and a tetranuclear Co(ii) Co(iii) mixed valence polynuclear one. The latter shows SMM behaviour revealed unde...
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| Vydáno v: | Dalton transactions : an international journal of inorganic chemistry Ročník 47; číslo 47; s. 17055 |
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| Hlavní autoři: | , , , , , , |
| Médium: | Journal Article |
| Jazyk: | angličtina |
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England
21.12.2018
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| ISSN: | 1477-9234, 1477-9234 |
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| Abstract | We report the synthesis, structural characterization and a combined computational and experimental study of the magnetic properties of two pivalate cobalt complexes, a mononuclear Co(ii) one and a tetranuclear Co(ii)
Co(iii) mixed valence polynuclear one. The latter shows SMM behaviour revealed under an applied DC field with a thermal barrier of ca. 30 cm
competing with direct and Raman relaxation processes. The Orbach thermal barrier can be understood from the doublets energy ladder arising from the anisotropic exchange interaction among ground S
= 1/2 of each Co(ii) sites. The strong local zero-field splitting of the S = 3/2 Co(ii) states affords these well isolated ground Kramers doublets. DC and AC magnetic susceptibility measurements as well as HF-EPR spectra support this interpretation. CASSCF quantum chemical computations have been also performed in order to aid the overall comprehension of the magnetic behaviour in the reported complexes. |
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| AbstractList | We report the synthesis, structural characterization and a combined computational and experimental study of the magnetic properties of two pivalate cobalt complexes, a mononuclear Co(ii) one and a tetranuclear Co(ii)3Co(iii) mixed valence polynuclear one. The latter shows SMM behaviour revealed under an applied DC field with a thermal barrier of ca. 30 cm-1 competing with direct and Raman relaxation processes. The Orbach thermal barrier can be understood from the doublets energy ladder arising from the anisotropic exchange interaction among ground Seff = 1/2 of each Co(ii) sites. The strong local zero-field splitting of the S = 3/2 Co(ii) states affords these well isolated ground Kramers doublets. DC and AC magnetic susceptibility measurements as well as HF-EPR spectra support this interpretation. CASSCF quantum chemical computations have been also performed in order to aid the overall comprehension of the magnetic behaviour in the reported complexes.We report the synthesis, structural characterization and a combined computational and experimental study of the magnetic properties of two pivalate cobalt complexes, a mononuclear Co(ii) one and a tetranuclear Co(ii)3Co(iii) mixed valence polynuclear one. The latter shows SMM behaviour revealed under an applied DC field with a thermal barrier of ca. 30 cm-1 competing with direct and Raman relaxation processes. The Orbach thermal barrier can be understood from the doublets energy ladder arising from the anisotropic exchange interaction among ground Seff = 1/2 of each Co(ii) sites. The strong local zero-field splitting of the S = 3/2 Co(ii) states affords these well isolated ground Kramers doublets. DC and AC magnetic susceptibility measurements as well as HF-EPR spectra support this interpretation. CASSCF quantum chemical computations have been also performed in order to aid the overall comprehension of the magnetic behaviour in the reported complexes. We report the synthesis, structural characterization and a combined computational and experimental study of the magnetic properties of two pivalate cobalt complexes, a mononuclear Co(ii) one and a tetranuclear Co(ii) Co(iii) mixed valence polynuclear one. The latter shows SMM behaviour revealed under an applied DC field with a thermal barrier of ca. 30 cm competing with direct and Raman relaxation processes. The Orbach thermal barrier can be understood from the doublets energy ladder arising from the anisotropic exchange interaction among ground S = 1/2 of each Co(ii) sites. The strong local zero-field splitting of the S = 3/2 Co(ii) states affords these well isolated ground Kramers doublets. DC and AC magnetic susceptibility measurements as well as HF-EPR spectra support this interpretation. CASSCF quantum chemical computations have been also performed in order to aid the overall comprehension of the magnetic behaviour in the reported complexes. |
| Author | Sarto, Carolina Bamberger, Heiko van Slageren, Joris Alborés, Pablo Rouzières, Mathieu Clérac, Rodolphe Liu, Jun-Liang |
| Author_xml | – sequence: 1 givenname: Carolina surname: Sarto fullname: Sarto, Carolina email: albores@qi.fcen.uba.ar organization: Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE (CONICET), Facultad de Ciencias Exactas y Naturales Universidad de Buenos Aires, Pabellón 2, Ciudad Universitaria, C1428EHA Buenos Aires, Argentina. albores@qi.fcen.uba.ar – sequence: 2 givenname: Mathieu surname: Rouzières fullname: Rouzières, Mathieu organization: CNRS, CRPP, UMR 5031, 33600 Pessac, France and Univ. Bordeaux, CRPP, UMR 5031, F-33600 Pessac, France – sequence: 3 givenname: Jun-Liang surname: Liu fullname: Liu, Jun-Liang organization: CNRS, CRPP, UMR 5031, 33600 Pessac, France and Univ. Bordeaux, CRPP, UMR 5031, F-33600 Pessac, France – sequence: 4 givenname: Heiko surname: Bamberger fullname: Bamberger, Heiko organization: Institut für Physikalische Chemie, Universität Stuttgart, Pfaffenwaldring 55, D-70569, Stuttgart, Germany – sequence: 5 givenname: Joris orcidid: 0000-0002-0855-8960 surname: van Slageren fullname: van Slageren, Joris organization: Institut für Physikalische Chemie, Universität Stuttgart, Pfaffenwaldring 55, D-70569, Stuttgart, Germany – sequence: 6 givenname: Rodolphe orcidid: 0000-0001-5429-7418 surname: Clérac fullname: Clérac, Rodolphe organization: CNRS, CRPP, UMR 5031, 33600 Pessac, France and Univ. Bordeaux, CRPP, UMR 5031, F-33600 Pessac, France – sequence: 7 givenname: Pablo orcidid: 0000-0002-6181-4521 surname: Alborés fullname: Alborés, Pablo email: albores@qi.fcen.uba.ar organization: Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE (CONICET), Facultad de Ciencias Exactas y Naturales Universidad de Buenos Aires, Pabellón 2, Ciudad Universitaria, C1428EHA Buenos Aires, Argentina. albores@qi.fcen.uba.ar |
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| Title | Slow magnetization dynamics in Co(ii)/Co(iii) triethanolamine/pivalate complexes |
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