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Title: 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:
 [1];  [2];  [2];  [3];  [4]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Univ. of Goettingen (Germany). Inst. of Inorganic Chemistry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  3. Univ. of California, Irvine, CA (United States). Dept. of Chemistry
  4. 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 Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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. doi: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. doi: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 = {2017},
month = {12}
}

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Cited by: 40 works
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Figures / Tables:

Fig. 1 Fig. 1: Synthesis and molecular structures of radical complexes. a Synthetic scheme for 1-Ln and 2-Ln. b Structure of the non-radical N22–-bridged complex 3-Ln, and structure of the N23− radical-bridged anions in crystals of 1-Ln and 2-Ln. Dark red, red, blue, and gray spheres represent Tb, O, N, and Cmore » atoms, respectively; H atoms have been omitted and THF groups faded for clarity. Selected interatomic distances (Å) and angles (deg) for 1-Gd, 1-Tb, and 1-Dy, respectively: N–N= 1.362(9), 1.371(6), 1.374(3); mean Ln–N= 2.288(8), 2.257(4), 2.236(2); Ln···Ln= 4.344(1), 4.294(3), 4.244(1); Ln–N–N–Ln= 173.3 (3), 173.4(3), 173.1(1). Selected interatomic distances (Å) for 2-Tb and 2-Dy, respectively: N–N= 1.392(9), 1.389(12); mean Ln–N= 2.221(6), 2.226(8); Ln···Ln= 4.216(1), 4.230(1); Ln–N–N–Ln= 178.3(3), 178.7(3)« less

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.