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Understanding the influence of dipolar interactions in magnetic hyperthermia (MH) experiments is of crucial importance for a fine optimization of nanoparticle (NP) heating power. In this study, we use a kinetic Monte-Carlo algorithm to calculate hyst eresis loops, so both time and temperature are correctly taken into account. It is demonstrated that this algorithm correctly reproduces the high-frequency hysteresis loop of both superparamagnetic NPs and ferromagnetic ones without any ad-hoc parameters. The algorithm is easily parallelizable so calculation on several processors decreases considerably calculation time. The specific absorption rate (SAR) of NPs dispersed inside spherical lysosomes is studied as a function of several key parameters: volume concentration, applied magnetic field, lysosome size, NP diameter and anisotropy. The influence of these parameters is illustrated and comprehensively explained. In summary, the effect of magnetic interactions is to increase the coercive field, saturation field and hysteresis area of major loops. However, for small amplitude magnetic field such as the ones used in MH, the heating power as function of concentration can increase, decrease or display a bell shape, depending of the relationship between the applied magnetic field and the coercive/saturation fields of the NPs. The hysteresis area is found to be well correlated to the parallel or antiparallel nature of the dipolar field acting on each NP. It is shown that the heating power increases or decreases sharply in the vicinity of the lysosome membrane. The amplitude of variation reaches more than one order of magnitude in certain conditions. Finally, implications of these various findings are discussed in the framework of MH optimization. It is concluded that feedbacks on specific points from biology experiments are required for further advance on the optimization of NPs for MH.
The influence of a transverse static magnetic field on the magnetic hyperthermia properties is studied on a system of large-losses ferromagnetic FeCo nanoparticles. The simultaneous measurement of the high-frequency hysteresis loops and of the temper ature rise provides an interesting insight into the losses and heating mechanisms. A static magnetic field of only 40 mT is enough to cancel the heating properties of the nanoparticles, a result reproduced using numerical simulations of hysteresis loops. These results cast doubt on the possibility to perform someday magnetic hyperthermia inside a magnetic resonance imaging setup.
To optimize the heating properties of magnetic nanoparticles (MNPs) in magnetic hyperthermia applications, it is necessary to calculate the area of their hysteresis loops in an alternating magnetic field. The three types of theories suitable for desc ribing the hysteresis loops of MNPs are presented and compared to numerical simulations: equilibrium functions, Stoner-Wohlfarth model based theories (SWMBTs) and linear response theory (LRT). Suitable formulas to calculate the hysteresis area of major cycles are deduced from SWMBTs and from numerical simulations; the domain of validity of the analytical formula is explicitly studied. In the case of minor cycles, the hysteresis area calculations are based on the LRT. A perfect agreement between LRT and numerical simulations of hysteresis loops is obtained. The domain of validity of the LRT is explicitly studied. Formulas to calculate the hysteresis area at low field valid for any anisotropy of the MNP are proposed. Numerical simulations of the magnetic field dependence of the area show it follows power-laws with a large range of exponents. Then, analytical expressions derived from LRT and SWMBTs are used for a theoretical study of magnetic hyperthermia. It is shown that LRT is only pertinent for MNPs with strong anisotropy and that SWMBTs should be used for weak anisotropy MNPs. The optimum volume of MNPs for magnetic hyperthermia as function of material and experimental parameters is derived. The maximum specific absorption rate (SAR) achievable is calculated versus the MNP anisotropy. It is shown that an optimum anisotropy increases the SAR and reduces the detrimental effects of size distribution. The optimum anisotropy is simple to calculate and depends on the magnetic field used in the hyperthermia experiments and on the MNP magnetization only. The theoretical optimum parameters are compared to the one of several magnetic materials.
We report on transport properties of millimetric super-lattices of CoFe nanoparticles surrounded by organic ligands. R(T)s follow R(T) = R_0.exp(T/T_0)^0.5 with T_0 ranging from 13 to 256 K. At low temperature I(V)s follow I=K[(V-V_T)/V_T]^ksi with k si ranging 3.5 to 5.2. I(V) superpose on a universal curve when shifted by a voltage proportional to the temperature. Between 1.8 and 10 K a high-field magnetoresistance with large amplitude and a strong voltage-dependence is observed. Its amplitude only depends on the magnetic field/temperature ratio. Its origin is attributed to the presence of paramagnetic states present at the surface or between the nanoparticles. Below 1.8 K, this high-field magnetoresistance abruptly disappears and inverse tunnelling magnetoresistance is observed, the amplitude of which does not exceed 1%. At this low temperature, some samples display in their I(V) characteristics abrupt and hysteretic transitions between the Coulomb blockade regime and the conductive regime. The increase of the current during these transitions can be as high as a factor 30. The electrical noise increases when the sample is near the transition. The application of a magnetic field decreases the voltage at which these transitions occur so magnetic-field induced transitions are also observed. Depending on the applied voltage, the temperature and the amplitude of the magnetic field, the magnetic-field induced transitions are either reversible or irreversible. These abrupt and hysteretic transitions are also observed in resistance-temperature measurements. They could be the soliton avalanches predicted by Sverdlov et al. [Phys. Rev. B 64, 041302 (R), 2001] or could also be interpreted as a true phase transition between a Coulomb glass phase to a liquid phase of electrons.
We report on hyperthermia measurements on a colloidal solution of 15 nm monodisperse FeCo nanoparticles (NPs). Losses as a function of the magnetic field display a sharp increase followed by a plateau, which is what is expected for losses of ferromag netic single-domain NPs. The frequency dependence of the coercive field is deduced from hyperthermia measurement and is in quantitative agreement with a simple model of non-interacting NPs. The measured losses (1.5 mJ/g) compare to the highest of the literature, though the saturation magnetization of the NPs is well below the bulk one.
We describe a low-cost and simple setup for hyperthermia measurements on colloidal solutions of magnetic nanoparticles (ferrofluids) with a frequency-adjustable magnetic field in the range 5-500 kHz produced by an electromagnet. By optimizing the gen eral conception and each component (nature of the wires, design of the electromagnet), a highly efficient setup is obtained. For instance, in a useful gap of 1.1 cm, a magnetic field of 4.8 mT is generated at 100 kHz and 500 kHz with an output power of 3.4 W and 75 W, respectively. A maximum magnetic field of 30 mT is obtained at 100 kHz. The temperature of the colloidal solution is measured using optical fiber sensors. To remove contributions due to heating of the electromagnet, a differential measurement is used. In this configuration the sensitivity is better than 1.5 mW at 100 kHz and 19.3 mT. This setup allows one to measure weak heating powers on highly diluted colloidal solutions. The hyperthermia characteristics of a solution of Fe nanoparticles are described, where both the magnetic field and the frequency dependence of heating power have been measured.
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