Incommensurate and commensurate antiferromagnetic states in CaMn2As2 and SrMn2As2 revealed by As75 NMR

Abstract

We carried out $^{75}\mathrm{As}$ nuclear magnetic resonance (NMR) measurements on the trigonal $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ and $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ insulators exhibiting antiferromagnetic (AFM) ordered states below N\'eel temperatures ${T}_{\mathrm{N}}=62$ and 120 K, respectively. In the paramagnetic state above ${T}_{\mathrm{N}}$, typical quadrupolar-split $^{75}\mathrm{As}$ NMR spectra were observed for both systems. The $^{75}\mathrm{As}$ quadrupolar frequency ${\ensuremath{\nu}}_{\mathrm{Q}}$ for $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ decreases with decreasing temperature, while ${\ensuremath{\nu}}_{\mathrm{Q}}$ for $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ increases, showing an opposite temperature dependence. In the AFM state, the relatively sharp and distinct $^{75}\mathrm{As}$ NMR lines were observed in $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ and the NMR spectra were shifted to lower fields for both magnetic fields $H\ensuremath{\parallel}c$ axis and $H\ensuremath{\parallel}ab$ plane, suggesting that the internal fields ${B}_{\mathrm{int}}$ at the As site produced by the Mn ordered moments are nearly perpendicular to the external magnetic field direction. No obvious distribution of ${B}_{\mathrm{int}}$ was observed in $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$, which clearly indicates a commensurate AFM state. In sharp contrast to $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$, broad and complex NMR spectra were observed in $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ in the AFM state, which clearly shows a distribution of ${B}_{\mathrm{int}}$ at the As site, indicating an incommensurate state. From the analysis of the characteristic shape of the observed spectra, the AFM state of $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ was determined to be a two-dimensional incommensurate state where Mn ordered moments are aligned in the $ab$ plane. A possible origin for the different AFM states in the systems was discussed. Both $\mathrm{Ca}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ and $\mathrm{Sr}{\mathrm{Mn}}_{2}{\mathrm{As}}_{2}$ show very large anisotropy in the nuclear spin-lattice relaxation rate $1/{T}_{1}$ in the paramagnetic state. $1/{T}_{1}$ for $H\ensuremath{\parallel}ab$ is much larger than that for $H\ensuremath{\parallel}c$, indicating strong anisotropic AFM spin fluctuations in both compounds.