Molecular intercalation in the van der Waals antiferromagnets FePS3 and NiPS3
Physical Review B(2024)
摘要
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 ^31P
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.
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