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oai:figshare.com:article/33814807 2026-09-15T18:02:01Z portal_1197 item_type_3 month_year_09_2026

Data for Emergent magnetic phases in pressure-tuned van der Waals antiferromagnet FePS3 Matthew John Coak (24935923) David M. Jarvis (24938995) Hayrullo Hamidov (2243032) Andrew R. Wildes (6489962) Joseph A. M. Paddison (9174601) Chengwei Liu (1530994) Charles R. S. Haines (24950314) Ngoc T. Dang (24950317) Sergey E. Kichanov (4033910) Boris N. Savenko (24950320) Sungmin Lee (166210) Marie Kratochvílová (24950323) Stefan Klotz (671224) Thomas C. Hansen (2117233) Denis P. Kozlenko (4033904) Je-Geun Park (1571797) Siddharth S. Saxena (7170938) Antiferromagnetism Magnetism Quasimolecules Monte Carlo method Pressure -- Measurement Migrated from ePrints Layered van-der-Waals 2D magnetic materials are of great interest in fundamental condensedmatter 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, 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.<br><br>The raw neutron diffraction data are hosted (permanently, and free to access, after a 12 month embargo) on the DOI archive of the Institut Laue Langevin: https://doi.ill.fr/10.5291/ill-data.5-31-2545 https://doi.ill.fr/10.5291/ill-data.5-31-2646 The reduced data - powder diffraction patterns - are included as tab-seperated data column text files in the Data files folder, with a spreadsheet explaining which measurement each corresponds to. Data are in 2theta, No of Counts, Error 3-column format. These are split between 3 folders - 2 for the experiments carried out at the ILL, and one for the data from Russia. Additionally, the results of the Reverse Monte Carlo simulations in Spinvert are included in the Simulation data folder, including the config files required to run the simulations. 2026-09-15T18:02:01Z Dataset Dataset 10.82444/warw.33814807.v1 https://figshare.com/articles/dataset/Data_for_Emergent_magnetic_phases_in_pressure-tuned_van_der_Waals_antiferromagnet_FePS3/33814807 CC BY 4.0