We report the growth of high-quality single crystals of ${\mathrm{ThCr}}_2{\mathrm{Si}}_2$-type tetragonal ${\mathrm{BaMn}}_2{\mathrm{P}}_2$ and investigation of its structural, electrical transport, thermal, and magnetic properties. Our results of basal plane electrical resistivity and heat capacity measurements show that the compound has an insulating ground state with a small band gap. Anisotropic susceptibility ${\chi }_{ab,c}\left(T\right)$ data infer a collinear local-moment Néel-type antiferromagnetic (AFM) ground state below the ordering temperature $T_{\mathrm{N}}=795\left(15\right)\mathrm{K}$, which is highest among all the ${\mathrm{ThCr}}_2{\mathrm{Si}}_2$- and ${\mathrm{CaAl}}_2{\mathrm{Si}}_2$-type 122-pnictide compounds reported so far suggesting that the strength of magnetic exchange interactions is strongest in this material. The magnetic transition temperatures of ${\mathrm{BaMn}}_{2}P{n}_2$ ($Pn=\mathrm{P}$, As, Sb, Bi) compounds exhibit a monotonic decrease with the increase of tetragonal unit cell parameters $a$ and $c$, suggesting a strong dependence of the strength of the decisive magnetic exchange interactions on the separation between the localized spins residing on the Mn ions. The observed monotonic increase of both ${\chi }_{ab}$ and ${\chi }_c$ for $T>T_{\mathrm{N}}$ suggests that short-range dynamic quasi-two-dimensional AFM correlations persist above the $T_{\mathrm{N}}$ up to the highest temperature of the measurements. The large $T_{\mathrm{N}}$ of ${\mathrm{BaMn}}_2{\mathrm{P}}_2$ demands for systematic hole-doping studies on this material as similar investigations on related ${\mathrm{BaMn}}_2{\mathrm{As}}_2$ with $T_{\mathrm{N}}=618\mathrm{K}$ have led to the discovery of an outstanding ground state where AFM of localized Mn spins and itinerant half-metallic ferromagnetism with $T_{\mathrm{c}}\approx 100\mathrm{K}$ originating from the doped holes coexist together.

• Received 22 February 2023
• Accepted 7 April 2023

DOI:https://doi.org/10.1103/PhysRevMaterials.7.044410