Journal
JOURNAL OF APPLIED PHYSICS
Volume 117, Issue 17, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/1.4919044
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Significant efforts towards understanding bi-magnetic core-shell nanoparticles are underway currently as they provide a pathway towards properties unavailable with single-phased systems. Recently, we have demonstrated that the magnetism of gamma-Fe2O3/CoO core-shell nanoparticles, in particular, at high temperatures, originates essentially from an interfacial doped iron-oxide layer that is formed by the migration of Co2+ from the CoO shell into the surface layers of the gamma-Fe2O3 core [Skoropata et al., Phys. Rev. B 89, 024410 (2014)]. To examine directly the nature of the intermixed layer, we have used high-resolution transmission electron microscopy (HRTEM) and first-principles calculations to examine the impact of the core-shell intermixing at the atomic level. By analyzing the HRTEM images and energy dispersive spectra, the level and nature of intermixing was confirmed, mainly as doping of Co into the octahedral site vacancies of gamma-Fe2O3. The average Co doping depths for different processing temperatures (150 degrees C and 235 degrees C) were 0.56 nm and 0.78 nm (determined to within 5% through simulation), respectively, establishing that the amount of core-shell intermixing can be altered purposefully with an appropriate change in synthesis conditions. Through first-principles calculations, we find that the intermixing phase of gamma-Fe2O3 with Co doping is ferromagnetic, with even higher magnetization as compared to that of pure gamma-Fe2O3. In addition, we show that Co doping into different octahedral sites can cause different magnetizations. This was reflected in a change in overall nanoparticle magnetization, where we observed a 25% reduction in magnetization for the 235 degrees C versus the 150 degrees C sample, despite a thicker intermixed layer. (C) 2015 AIP Publishing LLC.
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