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  Mössbauer Spectroscopy as a Probe of Magnetization Dynamics in the Linear Iron(I) and Iron(II) Complexes [Fe(C(SiMe3)3)2]1–/0

Zadrozny, J. M., Xiao, D. J., Long, J. R., Atanasov, M., Neese, F., Grandjean, F., et al. (2013). Mössbauer Spectroscopy as a Probe of Magnetization Dynamics in the Linear Iron(I) and Iron(II) Complexes [Fe(C(SiMe3)3)2]1–/0. Inorganic Chemistry, 52(22), 13123-13131. doi:10.1021/ic402013n.

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Zadrozny, Joseph M.1, Autor
Xiao, Dianne J.1, Autor
Long, Jeffrey R.1, Autor
Atanasov, Mihail2, 3, Autor           
Neese, Frank2, Autor           
Grandjean, Fernande4, Autor
Long, Gary J.4, Autor
Affiliations:
1Department of Chemistry, University of California, Berkeley, California 94720-1460, United States, ou_persistent22              
2Research Department Neese, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023886              
3 Institute of General and Inorganic Chemistry, Bulgarian Academy of Sciences, Acad. Georgi Bontchev Str 11, 1113 Sofia, Bulgaria, ou_persistent22              
4Department of Chemistry, Missouri University of Science and Technology, University of Missouri, Rolla, Missouri 65409-0010, United States, ou_persistent22              

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 Zusammenfassung: The iron-57 Mössbauer spectra of the linear, two-coordinate complexes, [K(crypt-222)][Fe(C(SiMe3)3)2], 1, and Fe(C(SiMe3)3)2, 2, were measured between 5 and 295 K under zero applied direct current (dc) field. These spectra were analyzed with a relaxation profile that models the relaxation of the hyperfine field associated with the inversion of the iron cation spin. Because of the lifetime of the measurement (10–8 to 10–9 s), iron-57 Mössbauer spectroscopy yielded the magnetization dynamics of 1 and 2 on a significantly faster time scale than was previously possible with alternating current (ac) magnetometry. From the modeling of the Mössbauer spectral profiles, Arrhenius plots between 5 and 295 K were obtained for both 1 and 2. The high-temperature regimes revealed Orbach relaxation processes with Ueff = 246(3) and 178(9) cm–1 for 1 and 2, respectively, effective relaxation barriers which are in agreement with magnetic measurements and supporting ab initio calculations. In 1, two distinct high-temperature regimes of magnetic relaxation are observed with mechanisms that correspond to two distinct single-excitation Orbach processes within the ground-state spin–orbit coupled manifold of the iron(I) ion. For 2, Mössbauer spectroscopy yields the temperature dependence of the magnetic relaxation in zero applied dc field, a relaxation that could not be observed with zero-field ac magnetometry. The ab initio calculated Mössbauer hyperfine parameters of both 1 and 2 are in excellent agreement with the observed hyperfine parameters.

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Sprache(n): eng - English
 Datum: 2013-08-052013-10-312013-11-18
 Publikationsstatus: Erschienen
 Seiten: 9
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/ic402013n
 Art des Abschluß: -

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Titel: Inorganic Chemistry
  Kurztitel : Inorg. Chem.
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Washington, DC : American Chemical Society
Seiten: - Band / Heft: 52 (22) Artikelnummer: - Start- / Endseite: 13123 - 13131 Identifikator: ISSN: 0020-1669
CoNE: https://pure.mpg.de/cone/journals/resource/0020-1669