Data for Local nuclear and magnetic order in the two-dimensional spin glass, Mn0.5Fe0.5PS3

Nuclear neutron scattering data reveal a random distribution of Mn2+ and Fe2+ ions within the honeycomb layers, which gives rise to a spin glass state through inducing competition between neighbouring exchange interactions, indicated in magnetic susceptibility data by a cusp at the glass transition, Tg = 35 K. Analysis of magnetic diffuse neutron scattering data collected for both single crystal and polycrystalline samples gives further insight into the origin of the spin glass phase, with spin correlations revealing a mixture of satisfied and unsatisfied correlations between magnetic moments within the honeycomb planes, which can be explained by considering the magnetic structures of the parent compounds, MnPS3 and FePS3.

We found that, on approaching Tg from above, an ensemble-averaged correlation length of ξ = 5.5(6) ˚A developed between satisfied correlations, and below Tg, the glassy behaviour gave rise to a distanceindependent correlation between unsatisfied moments. Correlations between the planes were found to be very weak, which mirrored our observations of rod-like structures parallel to the c* axis in our single crystal diffraction measurements, confirming the two-dimensional nature of Mn0.5Fe0.5PS3.<br><br>Data record consists of a zip archive containing the raw data organised according to directory and an accompanying readme file.