Collective magnetic response of inhomogeneous nanoisland FeNi films around the percolation transition

By using superconducting quantum interference device (SQUID) magnetometry, we investigated anisotropic high-field (H ? 7T) low-temperature (10 K) magnetization response of inhomogeneous nanoisland FeNi films grown by rf sputtering deposition on Sitall (TiO₂) glass substrates. In the grown FeNi films, the FeNi layer nominal thickness varied from 0.6 to 2.5 nm, across the percolation transition at the d _c ? 1.8 nm. We discovered that, beyond conventional spin-magnetism of Fe₂₁Ni₇₉ permalloy, the extracted out-of-plane magnetization response of the nanoisland FeNi films is not saturated in the range of investigated magnetic fields and exhibits paramagnetic-like behavior. We found that the anomalous out-of-plane magnetization response exhibits an escalating slope with increase in the nominal film thickness from 0.6 to 1.1 nm, however, it decreases with further increase in the film thickness, and then practically vanishes on approaching the FeNi film percolation threshold. At the same time, the in-plane response demonstrates saturation behavior above 1.5–2T, competing with anomalously large diamagnetic-like response, which becomes pronounced at high magnetic fields. It is possible that the supported-metal interaction leads to the creation of a thin charge-transfer (CT) layer and a Schottky barrier at the FeNi film/Sitall (TiO₂) interface. Then, in the system with nanoscale circular domains, the observed anomalous paramagnetic-like magnetization response can be associated with a large orbital moment of the localized electrons. In addition, the inhomogeneous nanoisland FeNi films can possess spontaneous ordering of toroidal moments, which can be either of orbital or spin origin. The system with toroidal inhomogeneity can lead to anomalously strong diamagnetic-like response. The observed magnetization response is determined by the interplay between the paramagnetic- and diamagnetic-like contributions.