Thickness-dependent magnetic order and phase transition in V₅S₈

V₅S₈ is an ideal candidate to explore the magnetism at the two-dimensional (2D) limit. A recent experiment has shown that the V₅S₈ thin films exhibit an antiferromagnetic (AFM) to ferromagnetic (FM) phase transition with reducing thickness. Here, for the first time, using density functional theory calculations, we report the antiferromagnetic order of bulk V₅S₈, which is consistent with the previous experiments. The specific antiferromagnetic order is reproduced when U _eff = 2 eV is applied on the intercalated vanadium atoms within LDA. We find that the origin of the magnetic ordering is from superexchange interaction. We also investigate the thickness-dependent magnetic order in V₅S₈ thin films. It is found that there is an antiferromagnetic to ferromagnetic phase transition when V₅S₈ is thinned down to 2.2 nm. The main magnetic moments of the antiferromagnetic and ferromagnetic states of the thin films are located on the interlayered vanadium atoms, which is the same as that in the bulk. Meanwhile, the strain in the thin films also influences the AFM–FM phase transition. Our results not only reveal the magnetic order and origin in bulk V₅S₈ and thin films, but also provide a set of parameters which can be used in future calculations. (paper)