We present a combined study of zero-field 51 V and 127 I NMR at ambient pressure and specific heat and magnetization measurements under pressure up to 2.08 GPa on bulk single crystals of the van-der-Waals ferromagnet VI3. At ambient pressure, our results consistently demonstrate that VI3 undergoes a structural transition at Ts ≈ 78 K, followed by two subsequent ferromagnetic transitions at TF M 1 ≈ 50 K and TF M 2 ≈ 36 K upon cooling. At lowest temperature (T < TF M 2), two magnetically-ordered V sites exist, whereas only one magnetically-ordered V site is observed for TF M 1 < T < TF M 2. Whereas TF M 1 is almost unaffected by external pressure, TF M 2 is highly responsive to pressure and merges with the TF M 1 line at p ≈ 0.6 GPa. At even higher pressures (p ≈ 1.25 GPa), the TF M 2 line merges with the structural transition at Ts which becomes moderately suppressed with p for p < 1.25 GPa. Taken together, our data point towards a complex magnetic structure and an interesting interplay of magnetic and structural degrees of freedom in VI3.
PACS numbers: xxxarXiv:1907.08550v1 [cond-mat.str-el]