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Molecular intercalation in the van der Waals antiferromagnets FePS3 and NiPS3
- Source :
- Physical Review B 109, 184407(2024)
- Publication Year :
- 2024
-
Abstract
- We have performed electrochemical treatment of the van der Waals antiferromagnetic materials FePS$_3$ and NiPS$_3$ with the ionic liquid EMIM-BF$_4$, achieving significant molecular intercalation. Mass analysis of the intercalated compounds, EMIM$_x$-FePS$_3$ and EMIM$_x$-NiPS$_3$, indicated respective intercalation levels, $x$, of approximately 27\% and 37\%, and X-ray diffraction measurements demonstrated a massive (over 50\%) enhancement of the $c$-axis lattice parameters. To investigate the consequences of these changes for the magnetic properties, we performed magnetic susceptibility and $^{31}$P nuclear magnetic resonance (NMR) studies of both systems. For EMIM$_x$-FePS$_3$, intercalation reduces the magnetic ordering temperature from $T_N = 120$~K to 78~K, and we find a spin gap in the antiferromagnetic phase that drops from 45~K to 30~K. For EMIM$_x$-NiPS$_3$, the ordering temperature is almost unaffected (changing from 148~K to 145~K), but a change towards nearly isotropic spin fluctuations suggests an alteration of the magnetic Hamiltonian. Such relatively modest changes, given that the huge extension of the $c$ axes is expected to cause a very strong suppression any interlayer interactions, point unequivocally to the conclusion that the magnetic properties of both parent compounds are determined solely by two-dimensional (2D), intralayer physics. The changes in transition temperatures and low-temperature spin dynamics in both compounds therefore indicate that intercalation also results in a significant modulation of the intralayer magnetic interactions, which we propose is due to charge doping and localization on the P sites. Our study offers chemical intercalation with ionic liquids as an effective method to control not only the interlayer but also the intralayer interactions in quasi-2D magnetic materials.
Details
- Database :
- arXiv
- Journal :
- Physical Review B 109, 184407(2024)
- Publication Type :
- Report
- Accession number :
- edsarx.2403.01714
- Document Type :
- Working Paper
- Full Text :
- https://doi.org/10.1103/PhysRevB.109.184407