Slow Magnetic Relaxations in Cobalt(II) Tetranitrate Complexes. Studies of Magnetic Anisotropy by Inelastic Neutron Scattering and High-Frequency and High-Field EPR Spectroscopy

Chen, Lei; Cui, Hui-Hui; Stavretis, Shelby E.; Hunter, Seth C.; Zhang, Yi-Quan; Chen, Xue-Tai; Sun, Yi-Chen; Wang, Zhenxing; Song, You; Podlesnyak, Andrey A.; Ouyang, Zhong-Wen; Xue, Zi-Ling

doi:10.1021/acs.inorgchem.6b01544

Title: Slow Magnetic Relaxations in Cobalt(II) Tetranitrate Complexes. Studies of Magnetic Anisotropy by Inelastic Neutron Scattering and High-Frequency and High-Field EPR Spectroscopy

Journal Article · Wed Dec 07 00:00:00 EST 2016 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.6b01544· OSTI ID:1341566

Chen, Lei ^[1]; Cui, Hui-Hui ^[1]; Stavretis, Shelby E. ^[2]; Hunter, Seth C. ^[2]; Zhang, Yi-Quan ^[3]; Chen, Xue-Tai ^[1]; Sun, Yi-Chen ^[4]; Wang, Zhenxing ^[4]; Song, You ^[1]; Podlesnyak, Andrey A. ^[5]; Ouyang, Zhong-Wen ^[4]; Xue, Zi-Ling ^[2]

Nanjing Univ. (China). Collaborative Innovation Center of Advanced Microstructures and School of Chemistry and Chemical Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Nanjing Normal Univ. (People's Republic of China). School of Physical Science and Technology
Huazhong Univ. of Science and Technology, Wuhan (People's Republic of China). Wuhan National High Magnetic Field Center
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division

We synthesized and studied three mononuclear cobalt(II) tetranitrate complexes (A)₂[Co(NO₃)₄] with different countercations, Ph₄P⁺ (1), MePh₃P⁺ (2), and Ph₄As⁺ (3), using X-ray single-crystal diffraction, magnetic measurements, inelastic neutron scattering (INS), high-frequency and high-field EPR (HF-EPR) spectroscopy, and theoretical calculations. Furthermore, the X-ray diffraction studies reveal that the structure of the tetranitrate cobalt anion varies with the countercation. 1 and 2 exhibit highly irregular seven-coordinate geometries, while the central Co(II) ion of 3 is in a distorted-dodecahedral configuration. The sole magnetic transition observed in the INS spectroscopy of 1–3 corresponds to the zero-field splitting (2(D² + 3E²)^1/2) from 22.5(2) cm^–1 in 1 to 26.6(3) cm^–1 in 2 and 11.1(5) cm^–1 in 3. The positive sign of the D value, and hence the easy-plane magnetic anisotropy, was demonstrated for 1 by INS studies under magnetic fields and HF-EPR spectroscopy. The combined analyses of INS and HF-EPR data yield the D values as +10.90(3), +12.74(3), and +4.50(3) cm^–1 for 1–3, respectively. Frequency- and temperature-dependent alternating-current magnetic susceptibility measurements reveal the slow magnetization relaxation in 1 and 2 at an applied dc field of 600 Oe, which is a characteristic of field-induced single-molecule magnets (SMMs). Finally, the electronic structures and the origin of magnetic anisotropy of 1–3 were revealed by calculations at the CASPT2/NEVPT2 level.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1341566

Journal Information:: Inorganic Chemistry, Vol. 55, Issue 24; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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CCDC 1422339: Experimental Crystal Structure Determination: PASCON11 : bis(tetraphenylarsonium) tetrakis(nitrato)-cobalt(ii) Chen, Lei; Cui, Hui-Hui; Stavretis, Shelby https://doi.org/10.5517/ccdc.csd.cc1jr1x7 The current record is supplemented by this dataset	dataset	September 2015
CCDC 1412396: Experimental Crystal Structure Determination: BAHDAS : bis(methyl(triphenyl)phosphonium) tetrakis(nitrato)-cobalt(ii) Chen, Lei; Cui, Hui-Hui; Stavretis, Shelby E. https://doi.org/10.5517/ccdc.csd.cc1jdq5t The current record is supplemented by this dataset	dataset	July 2015
CCDC 1507843: Experimental Crystal Structure Determination: BAHKIH : bis(tetraphenylphosphonium) tetrakis(nitrato)-cobalt(ii) dichloromethane solvate Chen, Lei; Cui, Hui-Hui; Stavretis, Shelby https://doi.org/10.5517/ccdc.csd.cc1mm13d The current record is supplemented by this dataset	dataset	October 2016