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Published April 10, 2019 | Submitted + Published + Supplemental Material
Journal Article Open

Dimensional crossover in a layered ferromagnet detected by spin correlation driven distortions

Abstract

Magneto-elastic distortions are commonly detected across magnetic long-range ordering (LRO) transitions. In principle, they are also induced by the magnetic short-range ordering (SRO) that precedes a LRO transition, which contains information about short-range correlations and energetics that are essential for understanding how LRO is established. However these distortions are difficult to resolve because the associated atomic displacements are exceedingly small and do not break symmetry. Here we demonstrate high-multipole nonlinear optical polarimetry as a sensitive and mode selective probe of SRO induced distortions using CrSiTe_3 as a testbed. This compound is composed of weakly bonded sheets of nearly isotropic ferromagnetically interacting spins that, in the Heisenberg limit, would individually be impeded from LRO by the Mermin-Wagner theorem. Our results show that CrSiTe_3 evades this law via a two-step crossover from two- to three-dimensional magnetic SRO, manifested through two successive and previously undetected totally symmetric distortions above its Curie temperature.

Additional Information

© 2019 The Author(s). This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. Received 05 February 2019; Accepted 22 March 2019; Published 10 April 2019. Data availability: The datasets generated are/or analyzed during the current study are available from the corresponding author on reasonable request. This work was supported by ARO MURI Grant No. W911NF-16-1-0361. 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). A.R. acknowledges support from the Caltech Prize Fellowship. The MRL Shared Experimental Facilities are supported by the MRSEC Program of the NSF under Award No. DMR 1720256; a member of the NSF-funded Materials Research Facilities Network. S.D.W. acknowledges support from the Nanostructures Cleanroom Facility at the California NanoSystems Institute (CNSI). We thank Tom Hogan for performing the dilatometry measurements and Liangbo Liang, David Mandrus, Jan Musfeldt, Kai Xiao, and Houlong Zhuang for helpful discussions. Author Contributions: A.R. and D.H. conceived the experiment. A.R. performed the optical measurements. A.R., D.H., and L.B. analysed the data. L.B. performed the classical Heisenberg model calculations. E.Z. and S.D.W. prepared and characterized the sample. A.R. and D.H. wrote the manuscript. The authors declare no competing interests.

Attached Files

Published - s41467-019-09663-3.pdf

Submitted - 1904.10460.pdf

Supplemental Material - 41467_2019_9663_MOESM1_ESM.pdf

Supplemental Material - 41467_2019_9663_MOESM2_ESM.docx

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Additional details

Created:
August 19, 2023
Modified:
October 20, 2023