Emergent Magnetic Phases and Piezomagnetic Effects in Mn$_x$Ni$_{1-x}$F$_2$ Thin Film Alloys

Abstract: The effect of random competing single-ion anisotropies in antiferromagnets was studied using epitaxial Mn$x$Ni${1-x}$F$2$ antiferromagnetic thin film alloys grown via molecular beam epitaxy. The crystal structure of this material is tetragonal for all values of $x$, and the Mn sites have a magnetic easy axis single-ion anisotropy while the Ni sites have an easy plane anisotropy perpendicular to the Mn easy axis. Crystallographic and magnetization measurements demonstrated that the thin film alloys were homogeneously mixed and did not phase-separate into their constituent parts. Pure MnF$_2$ thin films epitaxially grown on MgF$_2$ exhibited compressive strain along all three crystallographic axes which resulted in piezomagnetic effects. The piezomagnetism disappeared if the film was grown on a (MnNi)F$_2$ graded buffer layer. A mean-field theory fit to the transition temperature as a function of the Mn concentration $x$, which takes into account piezomagnetic effects, gave a magnetic exchange constant between Mn and Ni ions of $J{\text{MnNi}} = 0.305 \pm 0.003$~meV. Mean-field theory calculations also predicted the existence of an oblique antiferromagnetic phase in the Mn$x$Ni${1-x}$F$2$ alloy which agreed with the experimental data. A magnetic phase diagram for Mn$_x$Ni${1-x}$F$2$ thin film alloys was constructed and showed evidence for the existence of two unique magnetic phases, in addition to the ordinary antiferromagnetic and paramagnetic phases: an oblique antiferromagnetic phase, and an emergent magnetic phase proposed to be either a magnetic glassy phase or a helical phase. The phase diagram is quantitatively different from that of Fe$_x$Ni${1-x}$F$_2$ because of the much larger single-ion anisotropy of Fe$^{2+}$ compared to Mn$^{2+}$.