BiFeO 3 (BFO) nanoparticles (NPs) were synthesized using the sol-gel method at different calcination temperatures from 400 °C to 600 °C. XRD studies have confirmed that all BFO NPs show distorted rhombohedral crystals that match the R3c space group. We found evidence of local structural strain that develops with increasing particle size as suggested by TEM and Raman spectroscopy measurements. Magnetic measurements suggest that NPs have two distinct regimes: a ferromagnetic-like one at low temperatures and a superparamagnetic-like one at room temperature. The crossover temperature increases with NPs size, suggesting a size-dependent blocking magnetic regime. Similarly, local piezoelectric measurements at room temperature in single NP have confirmed a ferroelectric order with a NP size-dependent d 33 coefficient. An analysis of both the ferroelectric and the magnetic results suggest that ferromagnetism and ferroelectricity coexist at room temperature in NPs. Our results lead to the possibility of tailoring the ferroic order in multifunctional materials by means of NP size.

Multiferroic materials are at the core of voltage-controlled spintronic devices. Therefore, an understanding of the underlying electronic correlations and their effects associated with their complex energy landscape is an important and ongoing task. One key parameter in oxidebased perovskite multiferroics is their sensitivity to strain effects under confinement. Here, we report on the ferromagnetism induced by strain-engineering at the nanoscale on BiFeO 3 (BFO) nanoparticles. By controlling synthesis parameters, we were able to modify the BFO lattice parameters up to 0.15% and as a consequence, induce ferromagnetism in otherwise antiferromagnetic bulk BFO. In order to understand the driving mechanisms behind such an effect, we performed density functional theory calculations (DFT) using the BFO parameters obtained from the experiment. We found that small distortions of the structural lattice parameters of the order of 0.01% are sufficient to induce a significant spin imbalance close to the Fermi energy at the Fe sites. This may explain the appearance of weak ferromagnetism in strained BFO thin films reported earlier and offers a new route to novel voltage-controlled spintronic devices based on multiferroic materials.

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