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

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Title
Emergent Magnetic Phases in Pressure-Tuned van der Waals Antiferromagnet FePS3
Author(s)
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.; Sungmin Lee; Marie Kratochvílová; Klotz, Stefan; Hansen, Thomas C.; Kozlenko, Denis P.; Je-Geun Park; Saxena, Siddharth S.
Publication Date
2021-02
Journal
PHYSICAL REVIEW X, v.11, no.1, pp.1 - 13
Publisher
AMER PHYSICAL SOC
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, 1/2) 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.
URI
https://pr.ibs.re.kr/handle/8788114/9252
DOI
10.1103/PhysRevX.11.011024
ISSN
2160-3308
Appears in Collections:
Center for Correlated Electron Systems(강상관계 물질 연구단) > 1. Journal Papers (저널논문)
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