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Title: High-temperature magnetic blocking and magneto-structural correlations in a series of dysprosium( iii ) metallocenium single-molecule magnets

Abstract

A series of dysprosium(III) metallocenium salts, [Dy(CpiPr4R)2][B(C6F5)4] (R = H (1), Me (2), Et (3), iPr (4)), was synthesized by reaction of DyI3 with the corresponding known NaCpiPr4R (R = H, iPr) and novel NaCpiPr4R (R = Me, Et) salts at high temperature, followed by iodide abstraction with [H(SiEt3)2][B(C6F5)4]. Variation of the substituents in this series results in substantial changes in molecular structure, with more sterically-encumbering cyclopentadienyl ligands promoting longer Dy–C distances and larger Cp–Dy–Cp angles. Dc and ac magnetic susceptibility data reveal that these structural changes have a considerable impact on the magnetic relaxation behavior and operating temperature of each compound. In particular, the magnetic relaxation barrier increases as the Dy–C distance decreases and the Cp–Dy–Cp angle increases. An overall 45 K increase in the magnetic blocking temperature is observed across the series, with compounds 2–4 exhibiting the highest 100 s blocking temperatures yet reported for a single-molecule magnet. Compound 2 possesses the highest operating temperature of the series with a 100 s blocking temperature of 62 K. Concomitant increases in the effective relaxation barrier and the maximum magnetic hysteresis temperature are observed, with 2 displaying a barrier of 1468 cm-1 and open magnetic hysteresis as high as 72more » K at a sweep rate of 3.1 mT s-1. Magneto-structural correlations are discussed with the goal of guiding the synthesis of future high operating temperature DyIII metallocenium single-molecule magnets.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [2]; ORCiD logo [3];  [1]; ORCiD logo [4]; ORCiD logo [1]
  1. US Navy, Naval Air Warfare Center, Weapons Division, Research Department, Chemistry Division
  2. Department of Chemistry, University of California, Berkeley, Berkeley, USA
  3. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, USA
  4. Department of Chemistry, University of California, Berkeley, Berkeley, USA, 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); National Science Foundation (NSF)
OSTI Identifier:
1479158
Alternate Identifier(s):
OSTI ID: 1493250
Grant/Contract Number:  
AC02-05CH11231; CHE-1800252
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 9 Journal Issue: 45; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Randall McClain, K., Gould, Colin A., Chakarawet, Khetpakorn, Teat, Simon J., Groshens, Thomas J., Long, Jeffrey R., and Harvey, Benjamin G. High-temperature magnetic blocking and magneto-structural correlations in a series of dysprosium( iii ) metallocenium single-molecule magnets. United Kingdom: N. p., 2018. Web. doi:10.1039/C8SC03907K.
Randall McClain, K., Gould, Colin A., Chakarawet, Khetpakorn, Teat, Simon J., Groshens, Thomas J., Long, Jeffrey R., & Harvey, Benjamin G. High-temperature magnetic blocking and magneto-structural correlations in a series of dysprosium( iii ) metallocenium single-molecule magnets. United Kingdom. doi:10.1039/C8SC03907K.
Randall McClain, K., Gould, Colin A., Chakarawet, Khetpakorn, Teat, Simon J., Groshens, Thomas J., Long, Jeffrey R., and Harvey, Benjamin G. Wed . "High-temperature magnetic blocking and magneto-structural correlations in a series of dysprosium( iii ) metallocenium single-molecule magnets". United Kingdom. doi:10.1039/C8SC03907K.
@article{osti_1479158,
title = {High-temperature magnetic blocking and magneto-structural correlations in a series of dysprosium( iii ) metallocenium single-molecule magnets},
author = {Randall McClain, K. and Gould, Colin A. and Chakarawet, Khetpakorn and Teat, Simon J. and Groshens, Thomas J. and Long, Jeffrey R. and Harvey, Benjamin G.},
abstractNote = {A series of dysprosium(III) metallocenium salts, [Dy(CpiPr4R)2][B(C6F5)4] (R = H (1), Me (2), Et (3), iPr (4)), was synthesized by reaction of DyI3 with the corresponding known NaCpiPr4R (R = H, iPr) and novel NaCpiPr4R (R = Me, Et) salts at high temperature, followed by iodide abstraction with [H(SiEt3)2][B(C6F5)4]. Variation of the substituents in this series results in substantial changes in molecular structure, with more sterically-encumbering cyclopentadienyl ligands promoting longer Dy–C distances and larger Cp–Dy–Cp angles. Dc and ac magnetic susceptibility data reveal that these structural changes have a considerable impact on the magnetic relaxation behavior and operating temperature of each compound. In particular, the magnetic relaxation barrier increases as the Dy–C distance decreases and the Cp–Dy–Cp angle increases. An overall 45 K increase in the magnetic blocking temperature is observed across the series, with compounds 2–4 exhibiting the highest 100 s blocking temperatures yet reported for a single-molecule magnet. Compound 2 possesses the highest operating temperature of the series with a 100 s blocking temperature of 62 K. Concomitant increases in the effective relaxation barrier and the maximum magnetic hysteresis temperature are observed, with 2 displaying a barrier of 1468 cm-1 and open magnetic hysteresis as high as 72 K at a sweep rate of 3.1 mT s-1. Magneto-structural correlations are discussed with the goal of guiding the synthesis of future high operating temperature DyIII metallocenium single-molecule magnets.},
doi = {10.1039/C8SC03907K},
journal = {Chemical Science},
number = 45,
volume = 9,
place = {United Kingdom},
year = {2018},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
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DOI: 10.1039/C8SC03907K

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    Electronic structures of bent lanthanide(III) complexes with two N-donor ligands
    journal, January 2019

    • Nicholas, Hannah M.; Vonci, Michele; Goodwin, Conrad A. P.
    • Chemical Science, Vol. 10, Issue 45
    • DOI: 10.1039/c9sc03431e

    A stable dysprosium( iii ) complex with a terminal fluoride ligand showing high resolution luminescence and slow magnetic relaxation
    journal, January 2020

    • Ling, Bo-Kai; Zhai, Yuan-Qi; Han, Junbo
    • Dalton Transactions, Vol. 49, Issue 21
    • DOI: 10.1039/d0dt01146k

    Synthesis and characterisation of light lanthanide bis-phospholyl borohydride complexes
    journal, January 2020

    • Liu, Jingjing; Nodaraki, Lydia E.; Cobb, Philip J.
    • Dalton Transactions, Vol. 49, Issue 19
    • DOI: 10.1039/d0dt01241f

    Redox- and solvato-magnetic switching in a tetrathiafulvalene-based triad single-molecule magnet
    journal, January 2020

    • Pointillart, Fabrice; Flores Gonzalez, Jessica; Montigaud, Vincent
    • Inorganic Chemistry Frontiers
    • DOI: 10.1039/d0qi00319k

    Boosting axiality in stable high-coordinate Dy( iii ) single-molecule magnets
    journal, January 2019

    • Canaj, Angelos B.; Singh, Mukesh Kumar; Regincós Marti, Emma
    • Chemical Communications, Vol. 55, Issue 42
    • DOI: 10.1039/c9cc00965e

    Slow relaxation of magnetization in unprecedented Cu–Ln-Rad hetero-tri-spin chains constructed from multidentate nitronyl nitroxide
    journal, January 2019

    • Sun, Juan; Sun, Zan; Wang, Kang
    • Journal of Materials Chemistry C, Vol. 7, Issue 29
    • DOI: 10.1039/c9tc02410g