Magnetoelastic coupling, negative thermal expansion, and two-dimensional magnetic excitations in FeAs

Abstract

We present a temperature-dependent investigation of the local structure and magnetic dynamics of the FeAs binary. The magnetic susceptibility $\ensuremath{\chi}(T)$ result shows an anomalous broad feature up to 550 K, with \ensuremath{\chi} continuing to increase above the N\'eel antiferromagnetic ordering temperature (${T}_{\mathrm{N}}=70\phantom{\rule{0.16em}{0ex}}\mathrm{K}$), peaking at \ensuremath{\sim}250 K, then decreasing gently above. It is remarkable that this peak susceptibility temperature corresponds to the onset of anisotropic negative thermal expansion in both the $a$ and $c$ axes, suggesting that magnetic interactions are affecting the structure even well above the N\'eel point. A systematic investigation into local bonding correlations, from time-of-flight neutron pair distribution function analyses, shows the octahedral volume around each Fe site growing monotonically while adjacent octahedra tilt toward one another before relaxing away past this peak in the anomalous magnetic susceptibility. We use inelastic-neutron scattering to map spin-wave excitations in FeAs at temperatures above and below the ${T}_{\mathrm{N}}$. We find magnetic excitations near ${T}_{\mathrm{N}}$ to be very different from the excitations in the ground state at 1.5 K. Spin waves measured at 1.5 K are three dimensional (3D), however, in the vicinity of the magnetic transition, the magnetic fluctuations clearly indicate two-dimensional (2D) character in this intrinsically 3D crystal structure. Unlike the undoped 2D parents of iron-arsenide superconductors, where the magnetic correlations are considerably weaker along the $c$ axis than in the $\mathit{ab}$ plane, inelastic neutron scattering here shows that the spin fluctuations in the 3D FeAs binary are nearly 2D in the $\mathit{bc}$ plane at 90 K. These results demonstrate the importance of short-range correlations in understanding the magnetic properties of transition-metal binaries, and suggest how 2D excitations, even in a 3D structure, can potentially become a breeding ground for unconventional superconductivity.