Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 41, Pages 17286-17290Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja3077654
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Funding
- Singapore National Research Foundation [NRF-G-CRP 2007-05]
- National University of Singapore Academic Research Fund [R-143-000-295-305]
- Australia ARC [DP110105338]
- American National Science Foundation [MRI-0421366]
- U.S. DOE [DE-AC36-08GO28308]
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Even though metal organic frameworks (MOFs) derived from antiferromagnetic dimeric-Cu(II) building units and nonmagnetic molecular linkers are known to exhibit unexpected ferromagnetic behavior, a comprehensive understanding of the underlying mechanism remains elusive. Using a combined theoretical and experimental approach, here we reveal the origin of the long-range ferromagnetic coupling in a series of MOFs, constructed from antiferromagnetic dimeric-Cu(II) building blocks. Our studies show that the strong localization of copper vacancy states favors spontaneous spin polarization and formation of local moment. These copper vacancy-induced moments are coupled via the itinerant electrons in the conjugated aromatic linkers to establish a long-range ferromagnetic ordering. The proposed mechanism is supported by direct experimental evidence of copper vacancies and the magnetic hysteresis (M-H) loops.
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