We apply the concepts of stochastic thermodynamics combined with the transition state theory to develop a framework for evaluating local heat distributions across the assemblies of interacting magnetic nanoparticles (MP) subject to time-varying external magnetic fields. We show that additivity of entropy production in the particle state-space allows separating the entropy contributions and evaluating the heat produced by the individual MPs despite interactions. Using MP chains as a model system for convenience, without losing generality, we show that the presence of dipolar interactions leads to significant heat distributions across the chains. Our study also suggests that the typically used hysteresis loops cannot be used as a measure of energy dissipation at the local particle level within MP clusters, aggregates or assemblies, and explicit evaluation of entropy production based on appropriate theory, such as developed here, becomes necessary.
An efficient and safe hyperthermia cancer treatment requires the accurate control of the heating performance of magnetic nanoparticles, which is directly related to their size. However, in any particle system the existence of some size polydispersity is experimentally unavoidable, which results in a different local heating output and consequently a different hyperthermia performance depending on the size of each particle. With the aim to shed some light on this significant issue, we have used a Monte Carlo technique to study the role of size polydispersity in heat dissipation at both the local (single particle) and global (macroscopic average) levels. We have systematically varied size polydispersity, temperature and interparticle dipolar interaction conditions, and evaluated local heating as a function of these parameters. Our results provide a simple guide on how to choose, for a given polydispersity degree, the more adequate average particle size so that the local variation in the released heat is kept within some limits that correspond to safety boundaries for the average-system hyperthermia performance. All together we believe that our results may help in the design of more effective magnetic hyperthermia applications.
In the context of using magnetic nanoparticles for heat-mediated applications, the need of an accurate knowledge of the local (at the nanoparticle level) heat generation in addition to the usually studied global counterpart has been recently highlighted. Such a need requires accurate knowledge of the links among the intrinsic particle properties, system characteristics and experimental conditions. In this work we have investigated the role of the particles' anisotropy polydispersity in relation to the amplitude (H) of the AC magnetic field using a Monte Carlo technique. Our results indicate that it is better to use particles with large anisotropy for enhancing global heating, whereas for achieving homogeneous local heating it is better to use lower anisotropy particles. The latter ensures that most of the system undergoes major-loop hysteresis conditions, which is the key-point. This is equivalent to say that low-anisotropy particles (i.e. with less heating capability) may be better for accurate heat-mediated applications, which goes against some research trends in the literature that seek for large anisotropy (and hence heating) values.
Recent experiments on magnetic nanoparticle hyperthermia show that the heat dissipated by particles must be considered locally, instead of characterizing it as a global quantity. Here we show theoretically that the complex energy transfer between nanoparticles interacting via magnetic dipolar fields can lead to negative local hysteresis loops and does not allow the use of these local hysteresis loops as a temperature measure. Our model shows that interacting nanoparticles release heat not only when the nanoparticle magnetization switches between different energy wells, but also in the intrawell motion, when the effective magnetic field is changed because the magnetization of another particle has switched. The temperature dynamics has a highly nontrivial dependence on the amount of precession, which is controlled by the magnetic damping. Our results constitute a step forward in modelling of magnetic nanoparticles for hyperthermia and other heating applications.
In the magnetic fluid hyperthermia (MFH) research field, it is usually assumed that achieving a uniform temperature enhancement (ΔT) of the entire tumour is a key-point for treatment. However, various experimental works reported successful cell apoptosis via MFH without a noticeable ΔT of the system. A possible explanation of the success of these negligible-ΔT experiments is that a local ΔT restricted to the particle nanoenvironment (i.e. with no significant effect on the global temperature T) could be enough to trigger cell death. Shedding light on such a possibility requires accurate knowledge of heat dissipation at the local level in relation to the usually investigated global (average) one. Since size polydispersity is inherent to all synthesis techniques and the heat released is proportional to the particle size, heat dissipation spots with different performances - and thus different effects on the cells - will likely exist in every sample. In this work we aim for a double objective: (1) to emphasize the necessity to distinguish between the total dissipated heat and hyperthermia effectiveness, and (2) to suggest a theoretical approach on how to select, for a given size polydispersity, a more adequate average size so that most of the particles dissipate within a desired heating power range. The results are reported in terms of FeO nanoparticles as a representative example.
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