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Evidence for a Parity Broken Monoclinic Ground State in the S = 1/2 Kagomé Antiferromagnet Herbertsmithite

Laurita, N. J. and Ron, A. and Han, J. W. and Scheie, A. and Sheckelton, J. P. and Smaha, R. W. and He, W. and Wen, J.-J. and Lee, J. S. and Lee, Y. S. and Norman, M. R. and Hsieh, D. (2019) Evidence for a Parity Broken Monoclinic Ground State in the S = 1/2 Kagomé Antiferromagnet Herbertsmithite. . (Unpublished)

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Nearest-neighbor interacting S = 1/2 spins on the ideal Kagomé lattice are predicted to form a variety of novel quantum entangled states, including quantum spin-liquid (SL) and valence bond solid (VBS) phases. In real materials, the presence of additional perturbative spin interactions may further expand the variety of entangled states, which recent theoretical analyses show are identifiable through the spontaneous loss of particular discrete point group symmetries. Here we comprehensively resolve the ground state point group symmetries of the prototypical Kagomé SL candidate ZnCu₃(OH)₆Cl₂ (Herbertsmithite) using a combination of optical ellipsometry and wavelength-dependent multi-harmonic optical polarimetry. We uncover a subtle parity breaking monoclinic structural distortion at a temperature above the nearest-neighbor exchange energy scale. Surprisingly, the parity-breaking order parameter is dramatically enhanced upon cooling and closely tracks the build-up of nearest-neighbor spin correlations, suggesting that it is energetically favored by the SL state. The refined low temperature symmetry group greatly restricts the number of viable ground states, and, in the perturbative limit, points toward the formation of a nematic Z₂ striped SL ground state - a SL analogue of a liquid crystal.

Item Type:Report or Paper (Discussion Paper)
Related URLs:
URLURL TypeDescription Paper
Ron, A.0000-0002-1840-7824
Norman, M. R.0000-0002-9459-078X
Hsieh, D.0000-0002-0812-955X
Additional Information:This work was supported by an ARO PECASE award W911NF-17-1-0204. D.H. also acknowledges support for instrumentation from the David and Lucile Packard Foundation and from the Institute for Quantum Information and Matter, an NSF Physics Frontiers Center (PHY-1733907). N.J.L. acknowledges partial support from the IQIM Postdoctoral Fellowship. M.R.N. was supported by the Materials Science and Engineering Division, Basic Energy Sciences, Office of Science, U.S. DOE. J.W.H. and J.S.L. acknowledge support from the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning under contract No. 2018R1A2B2005331. Crystal growth and characterization was performed at Stanford University and SLAC and was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-76SF00515. Use of the Laue machine was supported through the Institute for Quantum Matter at Johns Hopkins University, by the U.S. Department of Energy, Division of Basic Energy Sciences, Grant DE-SC-0019331. A.S was supported through the Gordon and Betty Moore foundation under the EPIQS program GBMF4532. We thank H. Changlani, S. A. Kivelson, P. A. Lee, T. Senthil, and O. Tchernyshyov for helpful conversations. Author contributions: D.H., N.J.L and M.R.N conceived the experiment. N.J.L and A.R performed the non-linear harmonic generation measurements. J.W.H and J.S.L performed the ellipsometry measurements. A.S and N.J.L. performed the Laue diffraction measurements. J.P.S, R.W.S, W.H, J.J.W and Y.S.L prepared and characterized the sample. N.J.L and M.R.N analyzed the data. N.J.L, M.R.N, and D.H wrote the manuscript. The authors declare no competing financial interests.
Group:UNSPECIFIED, Institute for Quantum Information and Matter
Funding AgencyGrant Number
Army Research Office (ARO)W911NF-17-1-0204
David and Lucile Packard FoundationUNSPECIFIED
Institute for Quantum Information and Matter (IQIM)UNSPECIFIED
Department of Energy (DOE)DE-AC02-76SF00515
National Research Foundation of Korea2018R1A2B2005331
Department of Energy (DOE)DE-SC-0019331
Gordon and Betty Moore FoundationGBMF4532
Record Number:CaltechAUTHORS:20191218-130358489
Persistent URL:
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100353
Deposited By: Tony Diaz
Deposited On:18 Dec 2019 21:30
Last Modified:04 Jun 2020 10:14

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