Òscar Iglesias

Learning from Nature to Improve the Heat Generation of Iron-Oxide Nanoparticles for Magnetic Hyperthermia Applications

The performance of magnetic nanoparticles is intimately entwined with their structure, mean size and magnetic anisotropy. Besides, ensembles offer a unique way of engineering the magnetic response by modifying the strength of the dipolar interactions between particles. Here we report on an experimental and theoretical analysis of magnetic hyperthermia, a rapidly developing technique in medical research and oncology. Experimentally, we demonstrate that single-domain cubic iron oxide particles resembling bacterial magnetosomes have superior magnetic heating efficiency compared to spherical particles of similar sizes. Monte Carlo simulations at the atomic level corroborate the larger anisotropy of the cubic particles in comparison with the spherical ones, thus evidencing the beneficial role of surface anisotropy in the improved heating power. Moreover we establish a quantitative link between the particle assembling, the interactions and the heating properties. This knowledge opens new perspectives for improved hyperthermia, an alternative to conventional cancer therapies.

Finite-size and surface effects in maghemite nanoparticles: Monte Carlo simulations

Finite-size and surface effects in fine particle systems are investigated by Monte Carlo simulation of a model of a

Role of surface disorder on the magnetic properties and hysteresis of nanoparticles

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Magnetic domains and surface effects in hollow maghemite nanoparticles

(maghemite) single particle. Periodic boundary conditions for a large enough system have been used to simulate the bulk properties and the results compared with those for a spherical shaped particle with free boundaries to evidence the role played by the surface on the anomalous magnetic properties displayed by these systems at low temperatures. Several outcomes of the model are in qualitative agreement with the experimental findings. A reduction of the magnetic ordering temperature, spontaneous magnetization, and coercive field is observed as the particle size is decreased. Moreover, the hysteresis loops become elongated with high values of the differential susceptibility, resembling those from frustrated or disordered systems. These facts are a consequence of the formation of a surface layer with higher degree of magnetic disorder than the core, which, for small sizes, dominates the magnetization processes of the particle. However, in contradiction with the assumptions of some authors, our model does not predict the freezing of the surface layer into a spin-glass-like state. The results indicate that magnetic disorder at the surface simply facilitates the thermal demagnetization of the particle at zero field, while the magnetization is increased at moderate fields, since surface disorder diminishes ferrimagnetic correlations within the particle. The change in shape of the hysteresis loops with the particle size demonstrates that the reversal mode is strongly influenced by the reduced atomic coordination and disorder at the surface.

Magnetic nanoparticles with bulklike properties (invited)

We present the results of Monte Carlo simulations of a model of a single maghemite ferrimagnetic nanoparticle including radial surface anisotropy distinct from that in the core with the aim to clarify its role on the magnetization processes at low temperatures. The low-temperature equilibrium states are analysed and compared to those of a ferromagnetic particle with the same lattice structure. We have found that the formation of hedgehog-like structures due to increased surface anisotropy is responsible for a change in the reversal mechanism of the particles.

Microscopic origin of exchange bias in core/shell nanoparticles

In the present work, we investigate the magnetic properties of ferrimagnetic and non-interacting maghemite hollow nanoparticles obtained by the Kirkendall effect. From the experimental characterization of their magnetic behavior, we find that polycrystalline hollow maghemite nanoparticles exhibit low blocked-to-superparamagnetic transition temperatures, small magnetic moments, significant coercivities and irreversibility fields, and no magnetic saturation on external magnetic fields up to 5 T. These results are interpreted in terms of the microstructural parameters characterizing the maghemite shells by means of atomistic Monte Carlo simulations of an individual spherical shell. The model comprises strongly interacting crystallographic domains arranged in a spherical shell with random orientations and anisotropy axis. The Monte Carlo simulation allows discernment between the influence of the polycrystalline structure and its hollow geometry, while revealing the magnetic domain arranggement in the different temperataure regimes.

Magnetic relaxation in terms of microscopic energy barriers in a model of dipolar interacting nanoparticles

The magnetic behavior of Fe3� xO4 nanoparticles synthesized by either high-temperature decomposition of an organic iron precursor or low-temperature coprecipitation in aqueous conditions is compared. Transmission electron microscopy, x-ray absorption spectroscopy, x-ray magnetic circular dichroism, and magnetization measurements show that nanoparticles synthesized by thermal decomposition display high crystal quality and bulklike magnetic and electronic properties, while nanoparticles synthesized by coprecipitation show much poorer crystallinity and particlelike phenomenology, including reduced magnetization, high closure fields, and shifted hysteresis loops. The key role of the crystal quality is thus suggested, because particlelike behavior for particles larger than about 5 nm is observed only when the particles are structurally defective. These conclusions are supported by Monte Carlo simulations. It is also shown that thermal decomposition is capable of producing nanoparticles that, after further stabilization in physiological conditions, are suitable for biomedical applications such as magnetic resonance imaging or biodistribution studies. V C 2011 American Institute of Physics. [doi:10.1063/1.3559504]

Spin-glass-like freezing of inner and outer surface layers in hollow γ-Fe2O3 nanoparticles.

We report the results of Monte Carlo simulations with the aim to clarify the microscopic origin of exchange bias in the magnetization hysteresis loops of a model of individual core/shell nanoparticles. Increase of the exchange coupling across the core/shell interface leads to an enhancement of exchange bias and to an increasing asymmetry between the two branches of the loops which is due to different reversal mechanisms. A detailed study of the magnetic order of the interfacial spins shows compelling evidence that the existence of a net magnetization due to uncompensated spins at the shell interface is responsible for both phenomena and allows to quantify the loop shifts directly in terms of microscopic parameters with striking agreement with the macroscopic observed values.

Controlling exchange bias in Co?CoOx nanoparticles by oxygen content

The magnetic relaxation and hysteresis of a system of single domain particles with dipolar interactions are studied by Monte Carlo simulations. We model the system by a chain of Heisenberg classical spins with randomly oriented easy-axis and log-normal distribution of anisotropy constants interacting through dipole-dipole interactions. Extending the so-called

Morphology influence on nanoscale magnetism of Co nanoparticles: Experimental and theoretical aspects of exchange bias

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