Layered van der Waals (vdW) chalcogenides
of 3d transition
metals
are a rich source of two-dimensional (2D) nanomaterials, in which
atomically thin layers with the terminating chalcogen atoms exhibit
promising functionality for novel spintronic devices. Here, we report
on the synthesis, crystal growth, and magnetic properties of FeAl2Se4, MnAl2S4, and MnAl2Se4 ternary chalcogenides. Crystal structures are
probed by powder X-ray diffraction, Mössbauer spectroscopy,
and high-resolution transmission electron microscopy. We improve the
structural models of FeAl2Se4 and MnAl2S4 and show that isostructural MnAl2S4 and MnAl2Se4 crystallize in the centrosymmetric R3̅̅m space group. In the crystal
structure, transition metal and Al atoms mutually occupy the octahedral
and tetrahedral voids of four close-packing chalcogen layers terminated
by vdW gaps. The transition-metal atoms form a triangular arrangement
inside the close-packing layers. As a result, FeAl2Se4 and MnAl2S4 show no long-range magnetic
order in the studied temperature range. In the paramagnetic state,
Fe and Mn possess effective magnetic moments of 4.99(2) and 5.405(6)
μB, respectively. Furthermore, FeAl2Se4 enters a frozen spin-disordered state below 12 K.