Hyperfine interactions in MnAs studied by perturbed angular correlations of $\gamma$-rays using the probe $^{77}$Br $\rightarrow ^{77}$Se and first principles calculations for MnAs and other Mn pnictides

The MnAs compound shows a first-order transition at T$_{c}$≈ 42$^{\circ}$C, and a second-order transition at T$_{t}$ ≈120$^{\circ}$C. The first-order transition, with structural (hexagonal-orthorhombic), magnetic (FM-PM) and electrical conductivity changes, is associated to magnetocaloric, magnetoelastic, and magnetoresistance effects. We report a study in a large temperature range from −196$^{\circ}$C up to 140$^{\circ}$C, using the $\gamma\!-\!\gamma$ perturbed angular correlations method with the radioactive probe $^{77}$Br→$^{77}$Se, produced at the ISOLDE-CERN facility. The electric field gradients and magnetic hyperfine fields are determined across the first- and second-order phase transitions encompassing the pure and mixed phase regimes in cooling and heating cycles. The temperature irreversibility of the 1st order phase transition is seen locally, at the nanoscopic scale sensitivity of the hyperfine field, by its hysteresis, detailing and complementing information obtained with macroscopic measurements (magnetization and X-ray powder diffraction). To interpret the results, hyperfine parameters were obtained with first-principles spin-polarized density functional calculations using the generalized gradient approximation with the full potential (L)APW+lo method (Wien2k code) by considering the Se probe at both Mn and As sites. A clear assignment of the probe location at the As site is made and complemented with the calculated densities of states and local magnetic moments. We model electronic and magnetic properties of the chemically similar MnSb and MnBi compounds, complementing previous calculations.