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Reply to Zayed: Interplay of magnetism and structure in the Shastry–Sutherland model

Haravifard, S. and Banerjee, A. and van Wezel, J. and Silevitch, D. M. and dos Santos, António M. and Lang, J. C. and Kermarrec, E. and Srajer, G. and Gaulin, B. D. and Molaison, J. J. and Dabkowska, H. A. and Rosenbaum, T. F. (2015) Reply to Zayed: Interplay of magnetism and structure in the Shastry–Sutherland model. Proceedings of the National Academy of Sciences of the United States of America, 112 (5). E383-E384. ISSN 0027-8424. PMCID PMC4321251. doi:10.1073/pnas.1423100112.

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The connection between electronic and structural degrees of freedom—whether successive, coincident, or causal—suffuses the study of phase transitions. The Shastry–Sutherland model of a planar network of coupled spin dimers (1) and its physical realization in SrCu_2(BO_3)_2 (SCBO) provide a fundamental quantum mechanical test of this connection at the onset of antiferromagnetic order. We summarize in Fig. 1 the current understanding of SCBO’s phase diagram for T < 200 K and an intermediate pressure range of 3.5–6 GPa (2–4). At pressures below ∼4–5 GPa, SCBO has a tetragonal structure that hosts several low-temperature magnetic phases. Above this pressure, monoclinic distortions reduce the symmetry of the lattice. In ref. 2, we performed full structural refinements of X-ray and neutron scattering measurements to identify a change in space group at 5.5 GPa as a function of temperature (red circles in Fig. 1). This structural change coincides with the onset of antiferromagnetic ordering as a function of temperature, and we argue that this is not a coincidence but instead represents a cooperative effect between distortions of the lattice, the dimers tilting out of the plane, and the emergence of long-range magnetic order. In his comment on our work, Zayed (5) proposes an alternative scenario, in which the antiferromagnetic ordering onsets at lower pressure, within the tetragonal phase, and is then stabilized by the structural distortion associated with the monoclinic phase. He further speculates that this earlier onset may be associated with the dome in the phase boundary reported in ref. 4 (dark red region, Fig. 1).

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Silevitch, D. M.0000-0002-6347-3513
Additional Information:© 2015 National Academy of Sciences. Published online before print January 21, 2015. The work at the University of Chicago was supported by National Science Foundation Grant DMR-1206519. The work performed at the Advanced Photon Source was supported by the US Department of Energy (DOE) Office of Basic Energy Sciences under Contract DEAC02-06CH11357. The work performed at the Spallation Neutron Source was supported by the DOE Office of Basic Energy Sciences. Author contributions: S.H. and T.F.R. designed research; S.H., A.B., A.M.d.S., J.C.L., E.K., G.S., B.D.G., and J.J.M. performed research; S.H., B.D.G., and H.A.D. contributed new reagents/analytic tools; S.H., J.v.W., D.M.S., and T.F.R. analyzed data; and S.H., J.v.W., D.M.S., and T.F.R. wrote the paper. The authors declare no conflict of interest.
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Department of Energy (DOE)DEAC02-06CH11357
Issue or Number:5
PubMed Central ID:PMC4321251
Record Number:CaltechAUTHORS:20150202-073638831
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Official Citation:S. Haravifard, A. Banerjee, J. van Wezel, D. M. Silevitch, António M. dos Santos, J. C. Lang, E. Kermarrec, G. Srajer, B. D. Gaulin, J. J. Molaison, H. A. Dabkowska, and T. F. Rosenbaum Reply to Zayed: Interplay of magnetism and structure in the Shastry–Sutherland model PNAS 2015 112 (5) E383-E384; published ahead of print January 21, 2015, doi:10.1073/pnas.1423100112
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:54270
Deposited By: Tony Diaz
Deposited On:02 Feb 2015 17:51
Last Modified:10 Nov 2021 20:31

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