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Control of the third dimension in copper-based square-lattice antiferromagnets
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(2016) Control of the third dimension in copper-based square-lattice antiferromagnets. Physical Review B , 93 (9). pp. 1-17. 094430. doi:10.1103/PhysRevB.93.094430
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WRAP_ Goddard_Control_Dimension_ClO4PRB.pdf - Accepted Version - Requires a PDF viewer. Download (7Mb) | Preview |
Official URL: http://dx.doi.org/10.1103/PhysRevB.93.094430
Abstract
Using a mixed-ligand synthetic scheme, we create a family of quasi-two-dimensional antiferromagnets, namely, [Cu(HF2)(pyz)2]ClO4 [pyz = pyrazine], [CuL2(pyz)2](ClO4)2 [L = pyO = pyridine-N-oxide and 4-phpy-O = 4-phenylpyridine-N-oxide. These materials are shown to possess equivalent two-dimensional [Cu(pyz)2]2+ nearly square layers, but exhibit interlayer spacings that vary from 6.5713 to 16.777 Å, as dictated by the axial ligands. We present the structural and magnetic properties of this family as determined via x-ray diffraction, electron-spin resonance, pulsed- and quasistatic-field magnetometry and muon-spin rotation, and compare them to those of the prototypical two-dimensional magnetic polymer Cu(pyz)2(ClO4)2. We find that, within the limits of the experimental error, the two-dimensional, intralayer exchange coupling in our family of materials remains largely unaffected by the axial ligand substitution, while the observed magnetic ordering temperature (1.91 K for the material with the HF2 axial ligand, 1.70 K for the pyO and 1.63 K for the 4-phpy-O) decreases slowly with increasing layer separation. Despite the structural motifs common to this family and Cu(pyz)2(ClO4)2, the latter has significantly stronger two-dimensional exchange interactions and hence a higher ordering temperature. We discuss these results, as well as the mechanisms that might drive the long-range order in these materials, in terms of departures from the ideal S=1/2 two-dimensional square-lattice Heisenberg antiferromagnet. In particular, we find that both spin-exchange anisotropy in the intralayer interaction and interlayer couplings (exchange, dipolar, or both) are needed to account for the observed ordering temperatures, with the intralayer anisotropy becoming more important as the layers are pulled further apart.
| Item Type: | Journal Article | ||||||||||||||||||||||||
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| Subjects: | Q Science > QC Physics Q Science > QD Chemistry |
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| Divisions: | Faculty of Science > Physics | ||||||||||||||||||||||||
| Library of Congress Subject Headings (LCSH): | Crystal lattices, Antiferromagnetism | ||||||||||||||||||||||||
| Journal or Publication Title: | Physical Review B | ||||||||||||||||||||||||
| Publisher: | American Physical Society | ||||||||||||||||||||||||
| ISSN: | 2469-9969 | ||||||||||||||||||||||||
| Official Date: | 25 March 2016 | ||||||||||||||||||||||||
| Dates: |
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| Date of first compliant deposit: | 28 April 2016 | ||||||||||||||||||||||||
| Volume: | 93 | ||||||||||||||||||||||||
| Number: | 9 | ||||||||||||||||||||||||
| Number of Pages: | 17 | ||||||||||||||||||||||||
| Page Range: | pp. 1-17 | ||||||||||||||||||||||||
| Article Number: | 094430 | ||||||||||||||||||||||||
| DOI: | 10.1103/PhysRevB.93.094430 | ||||||||||||||||||||||||
| Status: | Peer Reviewed | ||||||||||||||||||||||||
| Publication Status: | Published | ||||||||||||||||||||||||
| Access rights to Published version: | Restricted or Subscription Access | ||||||||||||||||||||||||
| Grant number: | DMR-1306158 (NSF), DMR- 1157490 (NSF) | ||||||||||||||||||||||||
| RIOXX Funder/Project Grant: |
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