Multiple Incommensurate Magnetic States in the Kagome Antiferromagnet Na2Mn3Cl8

Abstract

The kagome lattice can host exotic magnetic phases arising from frustrated and competing magnetic interactions. However, relatively few insulating kagome materials exhibit incommensurate magnetic ordering. Here, we present a study of the magnetic structures and interactions of antiferromagnetic Na${}_2$Mn${}_3$Cl${}_8$ with an undistorted Mn${}^{2+}$ kagome network. Using neutron-diffraction and bulk magnetic measurements, we show that Na${}_2$Mn${}_3$Cl${}_8$ hosts two different incommensurate magnetic states, which develop at $T_{N1}=1.6$ K and $T_{N2}=0.6$ K. Magnetic Rietveld refinements indicate magnetic propagation vectors of the form $\mathbf{q}=(q_x,q_y,\frac{3}{2})$, and our neutron-diffraction data can be well described by cycloidal magnetic structures. By optimizing exchange parameters against magnetic diffuse-scattering data, we show that the spin Hamiltonian contains ferromagnetic nearest-neighbor and antiferromagnetic third-neighbor Heisenberg interactions, with a significant contribution from long-ranged dipolar coupling. This experimentally-determined interaction model is compared with density-functional-theory simulations. Using classical Monte Carlo simulations, we show that these competing interactions explain the experimental observation of multiple incommensurate magnetic phases and may stabilize multi-$\mathbf{q}$ states. Our results expand the known range of magnetic behavior on the kagome lattice.

13 pages, 8 figures