CsMn₄As₃: A layered tetragonal transition-metal pnictide compound with antiferromagnetic ground state

We report the synthesis and properties of a new layered tetragonal ternary compound CsMn$_4$As$_3$ (structure: KCu$_4$S$_3$-type, space group: $P4/mmm$, No. 123 and $Z = 2$). The material is a small band-gap semiconductor and exhibits an antiferromagnetic ground state associated with Mn spins. The compound exhibits a signature of a distinct magnetic moment canting event at 150(5)~K with a canting angle of $\approx 0.3^{\circ}$. Although, some features of the magnetic characteristics of this new compound are qualitatively similar to those of the related BaMn$_2$As$_2$, the underlying Mn sublattices of the two materials are quite different. While the Mn square-lattice layers in BaMn$_2$As$_2$ are equally spaced along the $c$-direction with the interlayer distance $d_{\rm L\,Ba} = 6.7341(4)$ Ang., the Mn sublattice forms bilayers in CsMn$_4$As$_3$ with the interlayer distance within a bilayer $d_{\rm L\,Cs} = 3.1661(6)$ Ang. and the distance between the two adjacent bilayers $d_{\rm B} = 7.290(6)$ Ang. This difference in the Mn sublattice is bound to significantly alter the energy balance between the $J_{1}$, $J_{2}$ and $J_{c}$ exchange interactions within the J1-J2-Jc model compared to that in BaMn$_2$As$_2$ and the other related 122 compounds including the well-known iron-arsenide superconductor parent compound BaFe$_2$As$_2$. Owing to the novelty of its transition metal sublattice, this new addition to the family of tetragonal materials related to the iron-based superconductors brings prospects for doping and pressure studies in the search of new superconducting phases as well as other exciting correlated-electron properties.