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

Coak, Matthew J., Jarvis, David M., Hamidov, Hayrullo, Wildes, Andrew R., Paddison, Joseph A. M., Liu, Cheng, 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. ISSN 2160-3308

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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 ultrahigh-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.

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Additional Information: Funding Information: This work was supported by the Institute for Basic Science (IBS) in Korea (Grant No. IBS-R009-G1). We also acknowledge support from Jesus College of the University of Cambridge and from the Engineering and Physical Sciences Research Council. The work was carried out with financial support from the Ministry of Education and Science of the Russian Federation in the framework of Increase Competitiveness Program of NUST MISiS (K2-2017-024). J.-G. P. was partially supported by the Leading Researcher Program of the National Research Foundation of Korea (Grant No. 2020R1A3B2079375). J. A. M. P.’s work at Oak Ridge National Laboratory (ORNL) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (analysis of magnetic diffuse scattering data) and by the Laboratory Directed Research and Development program of ORNL, managed by UT-Battelle, LLC for the U.S. Department of Energy (discussion of manuscript). This manuscript has been coauthored by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. J. A. M. P.’s preliminary work at Cambridge was supported by Churchill College, University of Cambridge. This research was supported by United Kingdom Research and Innovation Global Challenges Research Fund COMPASS Grant No. ES/P010849/1 and Cambridge Central Asia Forum, Jesus College, Cambridge. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. 681260).
Uncontrolled Keywords: physics and astronomy(all) ,/dk/atira/pure/subjectarea/asjc/3100
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Depositing User: LivePure Connector
Date Deposited: 21 Sep 2021 01:36
Last Modified: 20 Oct 2021 03:27
URI: https://ueaeprints.uea.ac.uk/id/eprint/81467
DOI: 10.1103/PhysRevX.11.011024

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