• Open Access

Emergent Magnetic Phases in Pressure-Tuned van der Waals Antiferromagnet FePS3

Matthew J. Coak, David M. Jarvis, Hayrullo Hamidov, Andrew R. Wildes, Joseph A. M. Paddison, Cheng Liu, Charles R. S. Haines, Ngoc T. Dang, Sergey E. Kichanov, Boris N. Savenko, Sungmin Lee, Marie Kratochvílová, Stefan Klotz, Thomas C. Hansen, Denis P. Kozlenko, Je-Geun Park, and Siddharth S. Saxena
Phys. Rev. X 11, 011024 – Published 5 February 2021

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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  • Received 9 April 2020
  • Revised 15 September 2020
  • Accepted 28 October 2020

DOI:https://doi.org/10.1103/PhysRevX.11.011024

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

Published by the American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Matthew J. Coak1,2,*, David M. Jarvis1, Hayrullo Hamidov1,3,4, Andrew R. Wildes5, Joseph A. M. Paddison6,1, Cheng Liu1, Charles R. S. Haines7,1, Ngoc T. Dang8,9, Sergey E. Kichanov10, Boris N. Savenko10, Sungmin Lee11,12, Marie Kratochvílová11,12,13, Stefan Klotz14, Thomas C. Hansen5, Denis P. Kozlenko10, Je-Geun Park11,12,15, and Siddharth S. Saxena1,4,†

  • 1Cavendish Laboratory, University of Cambridge, J. J. Thomson Avenue, Cambridge CB3 0HE, United Kingdom
  • 2Department of Physics, University of Warwick, Gibbet Hill Road, Coventry CV4 7AL, United Kingdom
  • 3Navoi State Mining Institute, 27 Galaba Avenue, Navoi, Uzbekistan
  • 4National University of Science and Technology “MISiS,” Leninsky Prospekt 4, Moscow 119049, Russia
  • 5Institut Laue-Langevin, 71 Avenue des Martyrs, 38000 Grenoble, France
  • 6Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
  • 7Department of Earth Sciences, University of Cambridge, Downing Street, Cambridge CB2 3EQ, United Kingdom
  • 8Institute of Research and Development, Duy Tan University, 550000 Da Nang, Vietnam
  • 9Faculty of Natural Sciences, Duy Tan University, 550000 Da Nang, Vietnam
  • 10Frank Laboratory of Neutron Physics, Joint Institute for Nuclear Research, 141980 Dubna, Russia
  • 11Center for Correlated Electron Systems, Institute for Basic Science, Seoul 08826, Republic of Korea
  • 12Department of Physics and Astronomy, Seoul National University, Seoul 08826, Republic of Korea
  • 13Faculty of Mathematics and Physics, Department of Condensed Matter Physics, Charles University, Prague, Czech Republic
  • 14Sorbonne Université, IMPMC, CNRS, UMR 7590, 4 Place Jussieu, 75252 Paris, France
  • 15Center for Quantum Materials, Seoul National University, Seoul 08826, Republic of Korea

  • *Corresponding author. matthew.coak@warwick.ac.uk
  • Corresponding author. sss21@cam.ac.uk

Popular Summary

Imagine using the same pencil for writing on paper as well as on a specially designed screen. Such a “magic material” could be mechanically flexible and form a new kind of circuit for storing information and performing computation. Welcome to the world of “magnetic graphene,” which also changes its properties drastically when put under pressure or strain. Here, we present the first high-pressure neutron study of an example of magnetic graphene, FePS3, which transitions from an insulator to a metal when compressed.

This class of magnetic materials offers new routes to understanding the physics of novel magnetic states and superconductivity. Through the deployment of revolutionary high-pressure techniques, we have unveiled the evolution of magnetic ordering in FePS3 through its insulator-metal transition and into the unconventional metallic state.

These first-of-their-kind measurements have uncovered exotic new states and behaviors. We suspect that this newly discovered high-pressure magnetic phase most likely forms a precursor to superconductivity.

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Vol. 11, Iss. 1 — January - March 2021

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