Molecular intercalation in the van der Waals antiferromagnets FePS3 and NiPS3
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arXiv
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2024
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| _version_ | 1866914783423365120 |
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| author | Li, Cong Hu, Ze Hou, Xiaofei Xu, Sheng Wu, Zhanlong Du, Kefan Li, Shuo Xu, Xiaoyu Chen, Ying Wang, Zeyu Mu, Tiancheng Xia, Tian-Long Guo, Yanfeng Normand, B. Yu, Weiqiang Cui, Yi |
| author_facet | Li, Cong Hu, Ze Hou, Xiaofei Xu, Sheng Wu, Zhanlong Du, Kefan Li, Shuo Xu, Xiaoyu Chen, Ying Wang, Zeyu Mu, Tiancheng Xia, Tian-Long Guo, Yanfeng Normand, B. Yu, Weiqiang Cui, Yi |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2403_01714 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Molecular intercalation in the van der Waals antiferromagnets FePS3 and NiPS3 Li, Cong Hu, Ze Hou, Xiaofei Xu, Sheng Wu, Zhanlong Du, Kefan Li, Shuo Xu, Xiaoyu Chen, Ying Wang, Zeyu Mu, Tiancheng Xia, Tian-Long Guo, Yanfeng Normand, B. Yu, Weiqiang Cui, Yi Strongly Correlated Electrons Materials Science 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. |
| title | Molecular intercalation in the van der Waals antiferromagnets FePS3 and NiPS3 |
| topic | Strongly Correlated Electrons Materials Science |
| url | https://arxiv.org/abs/2403.01714 |