Spectroscopic Investigation of a Metal-Metal-Bonded Fe 6 Single-Molecule Magnet with an Isolated S = 19 / 2 Giant-Spin Ground State
The metal-metal-bonded molecule [Bu N][( L) Fe (dmf) ] (Fe ) was previously shown to possess a thermally isolated spin = / ground state and found to exhibit slow magnetization relaxation below a blocking temperature of ∼5 K [ , , 13949-13956]. Here, we present a comprehensive spectroscopic investiga...
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Published in | Inorganic chemistry Vol. 60; no. 7; pp. 4610 - 4622 |
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Main Authors | , , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
United States
American Chemical Society (ACS)
05.04.2021
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Abstract | The metal-metal-bonded molecule [Bu
N][(
L)
Fe
(dmf)
] (Fe
) was previously shown to possess a thermally isolated spin
=
/
ground state and found to exhibit slow magnetization relaxation below a blocking temperature of ∼5 K [
,
, 13949-13956]. Here, we present a comprehensive spectroscopic investigation of this unique single-molecule magnet (SMM), combining ultrawideband field-swept high-field electron paramagnetic resonance (EPR) with frequency-domain Fourier-transform terahertz EPR to accurately quantify the spin Hamiltonian parameters of Fe
. Of particular importance is the near absence of a 4th-order axial zero-field splitting term, which is known to arise because of quantum mechanical mixing of spin states on account of the relatively weak spin-spin (superexchange) interactions in traditional polynuclear SMMs such as the celebrated Mn
-acetate. The combined high-resolution measurements on both powder samples and an oriented single crystal provide a quantitative measure of the isolated nature of the spin ground state in the Fe
molecule, as well as additional microscopic insights into factors that govern the quantum tunneling of its magnetization. This work suggests strategies for improving the performance of polynuclear SMMs featuring direct metal-metal bonds and strong ferromagnetic spin-spin (exchange) interactions. |
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AbstractList | The metal-metal-bonded molecule [Bu
N][(
L)
Fe
(dmf)
] (Fe
) was previously shown to possess a thermally isolated spin
=
/
ground state and found to exhibit slow magnetization relaxation below a blocking temperature of ∼5 K [
,
, 13949-13956]. Here, we present a comprehensive spectroscopic investigation of this unique single-molecule magnet (SMM), combining ultrawideband field-swept high-field electron paramagnetic resonance (EPR) with frequency-domain Fourier-transform terahertz EPR to accurately quantify the spin Hamiltonian parameters of Fe
. Of particular importance is the near absence of a 4th-order axial zero-field splitting term, which is known to arise because of quantum mechanical mixing of spin states on account of the relatively weak spin-spin (superexchange) interactions in traditional polynuclear SMMs such as the celebrated Mn
-acetate. The combined high-resolution measurements on both powder samples and an oriented single crystal provide a quantitative measure of the isolated nature of the spin ground state in the Fe
molecule, as well as additional microscopic insights into factors that govern the quantum tunneling of its magnetization. This work suggests strategies for improving the performance of polynuclear SMMs featuring direct metal-metal bonds and strong ferromagnetic spin-spin (exchange) interactions. Not provided. |
Author | Holldack, Karsten Hill, Stephen Anderton, Kevin J Krzystek, J Herrmann, Carmen Aliabadi, Azar Malbrecht, Brian J Schnegg, Alexander Greer, Samuel M Stoll, Stefan Nehrkorn, Joscha Betley, Theodore A |
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Snippet | The metal-metal-bonded molecule [Bu
N][(
L)
Fe
(dmf)
] (Fe
) was previously shown to possess a thermally isolated spin
=
/
ground state and found to exhibit... Not provided. |
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SubjectTerms | Chemistry |
Title | Spectroscopic Investigation of a Metal-Metal-Bonded Fe 6 Single-Molecule Magnet with an Isolated S = 19 / 2 Giant-Spin Ground State |
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