Whereas magnetic frustration is typically associated with local-moment magnets in special geometric arrangements, here we show that ${\mathrm{SrCo}}_2{\mathrm{As}}_2$ is a candidate for frustrated itinerant magnetism. Using inelastic neutron scattering (INS), we find that antiferromagnetic (AF) spin fluctuations develop in the square Co layers of ${\mathrm{SrCo}}_2{\mathrm{As}}_2$ below $T\approx 100$ K centered at the stripe-type AF propagation vector of $(\frac{1}{2},\frac{1}{2})$, and that their development is concomitant with a suppression of the uniform magnetic susceptibility determined via magnetization measurements. We interpret this switch in spectral weight as signaling a temperature-induced crossover from an instability toward ferromagnetism ordering to an instability toward stripe-type AF ordering on cooling, and show results from Monte-Carlo simulations for a $J_1-J_2$ Heisenberg model that illustrates how the crossover develops as a function of the frustration ratio $-J_1/\left(2J_2\right)$. By putting our INS data on an absolute scale, we quantitatively compare them and our magnetization data to exact-diagonalization calculations for the $J_1-J_2$ model [N. Shannon et al., Eur. Phys. J. B 38, 599 (2004).], and show that the calculations predict a lower level of magnetic frustration than indicated by experiment. We trace this discrepancy to the large energy scale of the fluctuations ($J_{\text{avg}}\gtrsim 75$ meV), which, in addition to the steep dispersion, is more characteristic of itinerant magnetism.

• Received 23 October 2018
• Revised 19 June 2019

DOI:https://doi.org/10.1103/PhysRevB.100.054411