Frustration driven magnetic correlations in the spin-$5/2$ triangular lattice antiferromagnet RbFe(HPO$_{3}$)$_{2}$

Abstract

A detailed study of the structural and magnetic properties of a spin-$5/2$ triangular lattice antiferromagnet RbFe(HPO$_{3}$)$_{2}$ is presented using x-ray diffraction, magnetization, heat capacity, and $^{31}$P nuclear magnetic resonance (NMR) experiments on a polycrystalline sample. The crystal structure features an equilateral triangular lattice of Fe$^{3+}$ ions. The thermodynamic measurements reveal the onset of a magnetic long-range order at $T_{\rm N1} \simeq 7.8$ K in zero-field, followed by another low temperature field induced ordering at $T_{\rm N2}$ in higher fields. The transition at $T_{\rm N1}$ is further confirmed from the NMR spin lattice relaxation measurements. The value of the frustration ratio ($f \simeq 7$) implies moderate spin frustration in the compound. The $^{31}$P NMR spectra exhibit two distinct spectral lines corresponding to two inequivalent phosphorus sites (P1 and P2), consistent with the crystal structure. The P1 site is strongly coupled with an isotropic hyperfine coupling of $A_{\rm hf}^{\rm iso} = 0.55(2)$ T/$\mu_{\rm B}$ while the P2 site is weakly coupled with $A_{\rm hf}^{\rm iso} = 0.25(3)$ T/$\mu_{\rm B}$ with the Fe$^{3+}$ ions. The magnetic susceptibility and NMR shift data are described well assuming a spin-$5/2$ isotropic triangular lattice antiferromagnetic model with an average exchange coupling of $J/k_{\rm B} = 2.8(2)$ K. Below $T_{\rm N1}$, the spectra evolve into a nearly rectangular powder pattern, indicating a commensurate antiferromagnetic type order. The $^{31}$P spin-lattice relaxation rate well below $T_{\rm N1}$ follows a $T^3$ temperature dependence, implying a two-magnon Raman scattering mechanism in the ordered state. Three well-defined phase regimes are clearly ascertained in the $H-T$ phase diagram, reflecting a weak magnetic anisotropy in the compound.