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Emergent magnetic phases in pressure-tuned van der Waals antiferromagnet FePS3

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Coak, Matthew John, Jarvis, David M., Hamidov, Hayrullo, Wildes, Andrew R., Paddison, Joseph A. M., Liu, Chengwei, Haines, Charles R. S., Dang, Ngoc T., Kichanov, Sergey E., Savenko, Boris N., Lee, Sungmin, Kratochvílová, Marie , Klotz, Stefan , Hansen, Thomas C., Kozlenko, Denis P., Park, Je-Geun and Saxena, Siddharth S. (2021) Emergent magnetic phases in pressure-tuned van der Waals antiferromagnet FePS3. Physical Review X, 11 (1). 011024 . doi:10.1103/PhysRevX.11.011024 ISSN 2160-3308.

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Official URL: https://doi.org/10.1103/PhysRevX.11.011024

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Abstract

Layered van-der-Waals 2D magnetic materials are of great interest in fundamental condensed-matter physics research, as well as for potential applications in spintronics and device physics. We present neutron powder diffraction data using new ultra-high-pressure techniques to measure the magnetic structure of Mott-insulating 2D honeycomb antiferromagnet FePS3 at pressures up to 183 kbar and temperatures down to 80 K. These data are complemented by high-pressure magnetometry and reverse Monte Carlo modeling of the spin configurations. As pressure is applied, the previously-measured ambient-pressure magnetic order switches from an antiferromagnetic to a ferromagnetic interplanar interaction, and from 2D-like to 3D-like character. The overall antiferromagnetic structure within the
ab planes, ferromagnetic chains antiferromagnetically coupled, is preserved, but the magnetic propagation vector is altered from k=0,1,12) to k=(0,1,0), a halving of the magnetic unit cell size. At higher pressures, coincident with the second structural transition and the insulator-metal transition in this compound, we observe a suppression of this long-range-order and emergence of a form of magnetic short-range order which survives above room temperature. Reverse Monte Carlo fitting suggests this phase to be a short-ranged version of the original ambient pressure structure - with the Fe moment size remaining of similar magnitude and with a return to antiferromagnetic interplanar correlations. The persistence of magnetism well into the HP-II metallic state is an observation in contradiction with previous x-ray spectroscopy results which suggest a spin-crossover transition.

Item Type: Journal Article
Subjects: Q Science > QA Mathematics
Q Science > QC Physics
Divisions: Faculty of Science, Engineering and Medicine > Science > Physics
Library of Congress Subject Headings (LCSH): Antiferromagnetism, Magnetism, Quasimolecules, Monte Carlo method, Pressure -- Measurement
Journal or Publication Title: Physical Review X
Publisher: American Physical Society
ISSN: 2160-3308
Official Date: 5 February 2021
Dates:
DateEvent
5 February 2021Published
28 October 2020Available
28 October 2020Accepted
Volume: 11
Number: 1
Article Number: 011024
DOI: 10.1103/PhysRevX.11.011024
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Open Access (Creative Commons)
Date of first compliant deposit: 3 November 2020
Date of first compliant Open Access: 5 March 2021
RIOXX Funder/Project Grant:
Project/Grant IDRIOXX Funder NameFunder ID
IBS-R009-G1Institute for Basic Sciencehttp://dx.doi.org/10.13039/501100010446
UNSPECIFIEDJesus College, University of Cambridgehttp://dx.doi.org/10.13039/501100000644
UNSPECIFIED[EPSRC] Engineering and Physical Sciences Research Councilhttp://dx.doi.org/10.13039/501100000266
K2-2017-024[MES] Ministry of Education and Science of the Russian Federationhttp://dx.doi.org/10.13039/501100003443
2020R1A3B2079375National Research Foundation of Koreahttp://dx.doi.org/10.13039/501100003725
UNSPECIFIED[DOE] U.S. Department of Energyhttp://dx.doi.org/10.13039/100000015
681260H2020 European Research Councilhttp://dx.doi.org/10.13039/100010663
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