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Control of the third dimension in copper-based square-lattice antiferromagnets

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Goddard, Paul, Singleton, John, Franke, Isabel, Möller, Johannes S., Lancaster, Tom, Steele, Andrew J., Topping, Craig V., Blundell, Stephen, Pratt, Francis L., Baines, C. et al.
(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 ISSN 2469-9969.

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Official URL: http://dx.doi.org/10.1103/PhysRevB.93.094430

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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
Subjects: Q Science > QC Physics
Q Science > QD Chemistry
Divisions: Faculty of Science, Engineering and Medicine > 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:
DateEvent
25 March 2016Published
30 January 2016Submitted
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
Date of first compliant deposit: 28 April 2016
Date of first compliant Open Access: 28 April 2016
Grant number: DMR-1306158 (NSF), DMR- 1157490 (NSF)
RIOXX Funder/Project Grant:
Project/Grant IDRIOXX Funder NameFunder ID
UNSPECIFIED[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
DMR-1306158National Science Foundationhttp://dx.doi.org/10.13039/100000001
DMR-1157490National Science FoundationUNSPECIFIED
UNSPECIFIEDFlorida. Department of Statehttps://viaf.org/viaf/139521689
Science in 100U.S. Department of Energyhttp://dx.doi.org/10.13039/100000015
UNSPECIFIEDScience and Technology Facilities Councilhttp://dx.doi.org/10.13039/501100000271
UNSPECIFIEDPaul Scherrer Instituthttp://dx.doi.org/10.13039/501100004219
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