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Register a new userControlling magnetisations reversal mechanism and hyperthermia efficiency in core/shell magnetic nanoparticles by tuning the interphase coupling
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Magnetic particle hyperthermia, in which colloidal nanostructures are exposed to an alternating magnetic field, is a promising approach to cancer therapy. Unfortunately, the clinical efficacy of hyperthermia has not yet been optimized. Consequently, routes to improve magnetic particle hyperthermia such as designing hybrid structures comprised from different phase materials are actively pursued. Here we demonstrate enhanced hyperthermia efficiency in relative large spherical Fe/Fe-oxide core/shell nanoparticles through the manipulation of interactions between the core and shell phases. Experimental results on exemplary samples with diameters in the range 30-80 nm indicated a direct correlation of hysteresis losses to the observed temperature elevation rate with a maximum efficiency of around 0.9 kW/g. The absolute particle size, the core/shell ratio, and the interposition of a thin wustite interlayer, are shown to have powerful effects on the specific absorption rate. By comparing our measurements to micromagnetic calculations we have unveiled topologically non-trivial magnetisation reversal modes under which interparticle interactions become negligible, aggregates formation is minimized, and the energy that is converted into heat is increased. This information has been overlooked till date and is in stark contrast to the existing knowledge on homogeneous particles.
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We present a systematic study of core-shell Au/Fe_3O_4 nanoparticles produced by thermal decomposition under mild conditions. The morphology and crystal structure of the nanoparticles revealed the presence of Au core of <d> = (6.9pm 1.0) nm surrounded by Fe_3O_4 shell with a thickness of ~3.5 nm, epitaxially grown onto the Au core surface. The Au/Fe_3O_4 core-shell structure was demonstrated by high angle annular dark field scanning transmission electron microscopy analysis. The magnetite shell grown on top of the Au nanoparticle displayed a thermal blocking state at temperatures below T_B = 59 K and a relaxed state well above T_B. Remarkably, an exchange bias effect was observed when cooling down the samples below room temperature under an external magnetic field. Moreover, the exchange bias field (H_{EX}) started to appear at T~40 K and its value increased by decreasing the temperature. This effect has been assigned to the interaction of spins located in the magnetically disordered regions (in the inner and outer surface of the Fe_3O_4 shell) and spins located in the ordered region of the Fe_3O_4 shell.
When magnetic nanoparticles (MNPs) are single-domain and magnetically independent, their magnetic properties and the conditions to optimize their efficiency in magnetic hyperthermia applications are now well-understood. However, the influence of magnetic interactions on magnetic hyperthermia properties is still unclear. Here, we report hyperthermia and high-frequency hysteresis loop measurements on a model system consisting of MNPs with the same size but a varying anisotropy, which is an interesting way to tune the relative strength of magnetic interactions. A clear correlation between the MNP anisotropy and the squareness of their hysteresis loop in colloidal solution is observed : the larger the anisotropy, the smaller the squareness. Since low anisotropy MNPs display a squareness higher than the one of magnetically independent nanoparticles, magnetic interactions enhance their heating power in this case. Hysteresis loop calculations of independent and coupled MNPs are compared to experimental results. It is shown that the observed features are a natural consequence of the formation of chains and columns of MNPs during hyperthermia experiments: in these structures, when the MNP magnetocristalline anisotropy is small enough to be dominated by magnetic interactions, the hysteresis loop shape tends to be rectangular, which enhance their efficiency. On the contrary, when MNPs do not form chains and columns, magnetic interactions reduces the hysteresis loop squareness and the efficiency of MNPs compared to independent ones. The present work should improve the understanding and interpretation of magnetic hyperthermia experiments.
We present an atomistic model of a single nanoparticle with core/shell structure that takes into account its lattice strucutre and spherical geometry, and in which the values of microscopic parameters such as anisotropy and exchange constants can be tuned in the core, shell and interfacial regions. By means of Monte Carlo simulations of the hysteresis loops based on this model, we have determined the range of microscopic parameters for which loop shifts after field cooling can be observed. The study of the magnetic order of the interfacial spins for different particles sizes and values of the interfacial exchange coupling have allowed us to correlate the appearance of loop asymmetries and vertical displacements to the existence of a fraction of uncompensated spins at the shell interface that remain pinned during field cycling, offering new insight on the microscopic origin of the experimental phenomenology.
We present a numerical simulation study of the exchange bias (EB) effect in nanoparticles with core/shell structure aimed to unveil the microscopic origin of some of the experimental phenomenology associated to this effect. In particular, we have focused our study on the particle size and field cooling dependence of the hysteresis loop shifts. To this end, hysteresis loops after a field cooling process have been computed by means of Monte Carlo simulations based on a model that takes into account the peculiar properties of the core, shell and interfacial regions of the particle and the EB and coercive fields have been extracted from them. The results show that, as a general trend, the EB field $h_{EB}$ decreases with increasing particle size, in agreement with some experimental observations. However, closer inspection reveals notable oscillations of $h_{EB}$ as a function of the particle radius which we show to be closely related to the net magnetization established after field cooling at the interfacial shell spins. For a particle with ferromagnetic interface coupling, we show that the magnitude and sign of $h_{EB}$ can be varied with the magnetic field applied during the cooling process.
We report on the magnetic and hyperthermia properties of iron nanoparticles synthesized by organometallic chemistry. They are 5.5 nm in diameter and display a saturation magnetization close to the bulk one. Magnetic properties are dominated by the contribution of aggregates of nanoparticles with respect to individual isolated nanoparticles. Alternative susceptibility measurements are been performed on a low interacting system obtained after eliminating the aggregates by centrifugation. A quantitative analysis using the Gittleman s model allow a determination of the effective anisotropy Keff = 1.3 * 10^5 J.m^{-3}, more than two times the magnetocristalline value of bulk iron. Hyperthermia measurements are performed on agglomerates of nanoparticles at a magnetic field up to 66 mT and at frequencies in the range 5-300 kHz. Maximum measured SAR is 280 W/g at 300 kHz and 66 mT. Specific absorption rate (SAR) displays a square dependence with the magnetic field below 30 mT but deviates from this power law at higher value. SAR is linear with the applied frequency for mu_0H=19 mT. The deviations from the linear response theory are discussed. A refined estimation of the optimal size of iron nanoparticles for hyperthermia applications is provided using the determined effective anisotropy value.
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