Giant coercivity and high magnetic blocking temperatures for N23- radical-bridged dilanthanide complexes upon ligand dissociation
Abstract
Increasing the operating temperatures of single-molecule magnets—molecules that can retain magnetic polarization in the absence of an applied field—has potential implications toward information storage and computing, and may also inform the development of new bulk magnets. Progress toward these goals relies upon the development of synthetic chemistry enabling enhancement of the thermal barrier to reversal of the magnetic moment, while suppressing alternative relaxation processes. Here in this paper, we show that pairing the axial magnetic anisotropy enforced by tetramethylcyclopentadienyl (CpMe4H) capping ligands with strong magnetic exchange coupling provided by an N23- radical bridging ligand results in a series of dilanthanide complexes exhibiting exceptionally large magnetic hysteresis loops that persist to high temperatures. Significantly, reducing the coordination number of the metal centers appears to increase axial magnetic anisotropy, giving rise to larger magnetic relaxation barriers and 100-s magnetic blocking temperatures of up to 20 K, as observed for the complex [K(crypt-222)][(CpMe4H2Tb)2(μ-N∙2
- Authors:
-
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Univ. of Goettingen (Germany). Inst. of Inorganic Chemistry
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
- Univ. of California, Irvine, CA (United States). Dept. of Chemistry
- Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1416939
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Coordination chemistry; Magnetic materials; Organometallic chemistry
Citation Formats
Demir, Selvan, Gonzalez, Miguel I., Darago, Lucy E., Evans, William J., and Long, Jeffrey R. Giant coercivity and high magnetic blocking temperatures for N23- radical-bridged dilanthanide complexes upon ligand dissociation. United States: N. p., 2017.
Web. doi:10.1038/s41467-017-01553-w.
Demir, Selvan, Gonzalez, Miguel I., Darago, Lucy E., Evans, William J., & Long, Jeffrey R. Giant coercivity and high magnetic blocking temperatures for N23- radical-bridged dilanthanide complexes upon ligand dissociation. United States. https://doi.org/10.1038/s41467-017-01553-w
Demir, Selvan, Gonzalez, Miguel I., Darago, Lucy E., Evans, William J., and Long, Jeffrey R. Fri .
"Giant coercivity and high magnetic blocking temperatures for N23- radical-bridged dilanthanide complexes upon ligand dissociation". United States. https://doi.org/10.1038/s41467-017-01553-w. https://www.osti.gov/servlets/purl/1416939.
@article{osti_1416939,
title = {Giant coercivity and high magnetic blocking temperatures for N23- radical-bridged dilanthanide complexes upon ligand dissociation},
author = {Demir, Selvan and Gonzalez, Miguel I. and Darago, Lucy E. and Evans, William J. and Long, Jeffrey R.},
abstractNote = {Increasing the operating temperatures of single-molecule magnets—molecules that can retain magnetic polarization in the absence of an applied field—has potential implications toward information storage and computing, and may also inform the development of new bulk magnets. Progress toward these goals relies upon the development of synthetic chemistry enabling enhancement of the thermal barrier to reversal of the magnetic moment, while suppressing alternative relaxation processes. Here in this paper, we show that pairing the axial magnetic anisotropy enforced by tetramethylcyclopentadienyl (CpMe4H) capping ligands with strong magnetic exchange coupling provided by an N23- radical bridging ligand results in a series of dilanthanide complexes exhibiting exceptionally large magnetic hysteresis loops that persist to high temperatures. Significantly, reducing the coordination number of the metal centers appears to increase axial magnetic anisotropy, giving rise to larger magnetic relaxation barriers and 100-s magnetic blocking temperatures of up to 20 K, as observed for the complex [K(crypt-222)][(CpMe4H2Tb)2(μ-N∙2},
doi = {10.1038/s41467-017-01553-w},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {Fri Dec 15 00:00:00 EST 2017},
month = {Fri Dec 15 00:00:00 EST 2017}
}
Web of Science
Figures / Tables:
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From zero-dimensional to one-dimensional chain N -oxide bridged compounds with enhanced single-molecule magnetic performance
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Synthesis of a series of hetero-multi-spin Ln 2 Cu 3 complexes based on a methyl-pyrazole nitronyl nitroxide radical with slow magnetic relaxation behaviors
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Tetraoxolene-bridged rare-earth complexes: a radical-bridged dinuclear Dy single-molecule magnet
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A family of lanthanide complexes with a bis-tridentate nitronyl nitroxide radical: syntheses, structures and magnetic properties
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Linear hexanuclear helical dysprosium single-molecule magnets: the effect of axial substitution on magnetic interactions and relaxation dynamics
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Regulating the structural dimensionality and dynamic properties of a porous dysprosium coordination polymer through solvent molecules
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Slow relaxation of magnetization in unprecedented Cu–Ln-Rad hetero-tri-spin chains constructed from multidentate nitronyl nitroxide
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Slow magnetic dynamics in centrosymmetric didysprosium and equilateral triangular tridysprosium molecules
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Synergistic effect of mixed ligands on the anisotropy axis of two dinuclear dysprosium complexes
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Slow relaxation of magnetization for a Tb derivative in a biradical-based lanthanide chain
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Magnetic hysteresis up to 80 kelvin in a dysprosium metallocene single-molecule magnet
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Bis(triphenylphosphine)iminium Salts of Dioxothiadiazole Radical Anions: Preparation, Crystal Structures, and Magnetic Properties
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Hohe Block‐Temperatur der Magnetisierung und herausragende Koerzitivfeldstärke im Azafulleren Tb 2 @C 79 N mit einer Einelektronen‐Terbium‐Terbium‐Bindung
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Magnetization Blocking in Fe 2 III Dy 2 III Molecular Magnets: Ab Initio Calculations and EPR Spectroscopy
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Magnetic Properties of Ln III -Cu II 15-Metallacrown-5 Dimers with Terephthalate (Ln III = Pr, Nd, Sm, Eu) : Magnetic Properties of Ln
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A family of multi-spin rare-earth complexes based on a triazole nitronyl nitroxide radical: synthesis, structure and magnetic properties
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Regulating the single-molecule magnetic properties of phenol oxygen-bridged binuclear lanthanide complexes through the electronic and spatial effect of the substituents
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Enhanced Selectivity for Oriented Catalyzing Tetracycline by the Functional Inorganic Imprinted ZnFe 2 O 4 @Ag 3 PO 4 /SiO 2 Photocatalyst with Excellent Stability
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Air-stable redox-active nanomagnets with lanthanide spins radical-bridged by a metal–metal bond
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Boosting axiality in stable high-coordinate Dy(III) single-molecule magnets
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A Redox-Active Bridging Ligand to Promote Spin Delocalization, High-Spin Complexes, and Magnetic Multi-Switchability
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High Blocking Temperature of Magnetization and Giant Coercivity in the Azafullerene Tb 2 @C 79 N with a Single-Electron Terbium–Terbium Bond
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Single-Electron Lanthanide-Lanthanide Bonds Inside Fullerenes toward Robust Redox-Active Molecular Magnets
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Lanthanide(III)-Based Single-Ion Magnets
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Air-stable redox-active nanomagnets with lanthanide spins radical-bridged by a metal–metal bond
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