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          Institute: MPI für bioanorganische Chemie     Collection: MPI für bioanorganische Chemie     Display Documents



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ID: 683899.0, MPI für bioanorganische Chemie / MPI für bioanorganische Chemie
Mössbauer Spectroscopy as a Probe of Magnetization Dynamics in the Linear Iron(I) and Iron(II) Complexes [Fe(C(SiMe 3)3)2]1-/0
Authors:Zadrozny, Joseph M.; Xiao, Dianne J.; Long, Jeffrey R.; Atanasov, Mihail; Neese, Frank; Grandjean, Fernande; Long, Gary J.
Language:English
Date of Publication (YYYY-MM-DD):2013
Title of Journal:Inorganic Chemistry
Journal Abbrev.:Inorg. Chem.
Volume:52
Start Page:13123
End Page:13131
Review Status:Peer-review
Audience:Experts Only
Abstract / Description:The iron-57 Mossbauer 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 Mossbauer 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 Mossbauer 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 U-eff = 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, Mossbauer 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 Mossbauer hyperfine parameters of both 1 and 2 are in excellent agreement with the observed hyperfine parameters.
External Publication Status:published
Document Type:Article
Communicated by:N. N.
Affiliations:MPI für bioanorganische Chemie
External Affiliations:Zadrozny, J.M.; Xiao, D.J.; Long, J.R.; Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA.;
Grandjean, F.; Long, G.J.; Univ Missouri, Missouri Univ Sci & Technol, Dept Chem, Rolla, MO 65409 USA.
Identifiers:ISI:000327225900035 [ID No:1]
ISSN:0020-1669 [ID No:2]
DOI:10.1021/ic402013n
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