Structural, Magnetic and Electronic Properties of Nanostructured Magnetic Materials
Authors:   , Prakash Tushara 
Published: November 2021

<p>This thesis was motivated by the different properties exhibited by magnetic nanoparticles when compared with the bulk. For example the coercivity and magnetocrystalline anisotropy vary with the particle size and the finite particle size can affect the spin-wave dispersion. When the nanoparticle radius becomes small enough it is possible to observe superparamagnetism with negligible hysteresis. The transport properties can also be different in nanoparticle composites when compared with the bulk. It is particularly interesting if the nanoparticles have a degree of electronic spin polarization because it is then possible to observe spin-dependent tunnelling. This thesis reports the results from a study of the structural, magnetic, and electronic properties of two partially electronically spin-polarized nanostructured compounds, iron-nickel alloy and magnetite, that were made using a new arc-discharge method, ion implantation and annealing, and a co-precipitation method.  It was found that permalloy powders could be made by arc-discharge where there were a range of particle sizes from nms to 10s of microns. Magnetoresistance was observed where it is due to the ordinary magnetoresistance and spin-dependent tunnelling between the particles. It was also possible to make magnetite using the arc-discharge process and the powders contained nanoparticles, large faceted nanoparticles, and larger particles in the 10s of micron range. The temperature dependence of the saturation magnetization changes at 127 K, which can be attributed to the charge-ordering Verwey transition. A large magnetoresistance was observed and attributed to spin-dependent tunnelling between the magnetite particles. It was less than predicted due to a spin-disordered interfacial region. The electrical resistance was modelled in terms of small nanoparticles coating the larger particles and electrostatic charging during tunnelling between small nanoparticles. Magnetite powders were also synthesized via a chemical co-precipitation method where nanoparticles with diameters of ~14 nm were observed. The Verwey transition was only observed in the zero-field cooled field-cooled magnetization for the arc-discharge powders. It was observed for the magnetite powders made using both methods in the temperature dependence of the saturation moment. The saturation magnetic moment for powders made using both methods has a power law dependence on temperature with an exponent of 3/2 at low temperatures and a higher value above the Verwey transition temperature 2. There was also a large magnetoresistance due to spin-dependent tunnelling for magnetite nanoparticle made using a chemical co-precipitation method and the electrical resistance could be modelled in terms of electrostatic charging during tunnelling.  NixFe₁₋x nanoparticles were made for the first time by ion beam implantation. Small superparamagnetic nanoparticles occurred after implantation. The saturation moment after implantation did not follow the Bloch’s T³/² for x=0.82, which is likely to be due to spin-waves propagating in the nanoparticle/NiyFe₁₋ySizOn matrix. A bi-modal particle size distribution of mostly spherical nanoparticles was observed for x=0.82 after annealing. An x=0.45 sample showed large asymmetric NixFe₁₋x nanoparticles with minimal smaller nanoparticles. The different nanoparticle morphologies is likely to be due to the different nucleation centres and the different initial concentration profiles. The saturation moment had an exponent of 3/2 at low temperatures and there was a contribution from surface disordered spins. A higher Ni fluence with x=0.53 lead to the formation of superparamagnetic nanoparticles that had a higher blocking temperature, indicating the formation of larger nanocrystallites. There was an enhancement in the permeability.</p>