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The relationship between vacancy ordering and magnetism in TlFe1.6Se2 hasbeen investigated via single crystal neutron diffraction, nuclear forwardscattering, and transmission electron microscopy. The examination of chemicallyand structurally homogenous crystals allows the true ground state to berevealed, which is characterized by Fe moments lying in the ab-plane below100K. This is in sharp contrast to crystals containing regions of order anddisorder, where a competition between c-axis and ab-plane orientations of themoments is observed. The properties of partially-disordered TlFe1.6Se2 aretherefore not associated with solely the ordered or disordered regions. Thiscontrasts the viewpoint that phase separation results in independent physicalproperties in intercalated iron selenides, suggesting a coupling betweenordered and disordered regions may play an important role in thesuperconducting analogues.

Spin reorientation in TlFe1.6Se2 with complete vacancy ordering