Local order in layered NiPS3 and Ni0.7Mg0.3PS3.

ABSTRACT

The family of two-dimensional magnetic materials M(II)PS(3) where M = Mn, Fe, Ni, Mg, Zn, etc shows a wide range of fascinating magnetic behaviour. It also shows potentially useful chemical properties including intercalation of nonlinear optical molecules and lithium ions. These properties are due to a crystal structure in which the ab planes are well-ordered in the plane but poorly correlated along c. Here, the short-range ordering is modelled in NiPS(3) and Ni(1 - x)Mg(x)PS(3) (x = 0.3). X-ray diffuse scattering from NiPS(3) shows pronounced streaking along c, indicative of stacking faulting in these layered compounds. Electron diffraction from Ni(1 - x)Mg(x)PS(3) (x = 0.3) shows substantial diffuse scattering due to short-range order within the ab plane, and this can be modelled by allowing the metal species to cluster. The possibility of clustering has implications for interpretation of the magnetic behaviour of the family, including the glassiness observed in Fe(1 - x)Mn(x)PS(3).