Ground-state properties of the $S=3/2$ anisotropic triangular lattice antiferromagnet Na$_3$Cr(PO$_4$)$_2$

Abstract

We report the crystal structure and magnetic properties of a $S=3/2$ anisotropic triangular lattice compound Na$_3$Cr(PO$_4$)$_2$ employing single-crystal and powder x-ray diffraction, magnetization, heat capacity, and $^{31}$P nuclear magnetic resonance (NMR) experiments, supported by the band structure calculations. Magnetic susceptibility exhibits a broad maximum around 3.5 K, indicating the presence of a short-range antiferromagnetic order, typical of a low-dimensional spin system. Magnetization and heat capacity manifest an antiferromagnetic long-range ordering at around $T_{\rm N} \simeq 2.6$ K. This was further confirmed by the drastic NMR line broadening and a peak in the nuclear spin-lattice and spin-spin relaxation rates. The isothermal magnetization data exhibit a field-induced spin-flop transition at around $μ_0H_{\rm SF} \simeq 1.7$ T reminiscent of an anisotropic two-dimensional magnet, before saturating above $μ_0H_{\rm sat} \simeq 4.5$ T. The saturation field was further upheld by the field-dependent NMR relaxation measurements at low temperatures. The $^{31}$P NMR spectral shape confirms the commensurate antiferromagnetic nature of the ordering below $T_{\rm N}$. \textit{Ab initio} calculations reveal a significant deformation of the triangular spin lattice, resulting in triangles with two antiferromagnetic couplings of similar strength and a much weaker coupling along the third side of the triangle.