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Register a new userTo Heat or not to Heat: a Study of the Performances of Iron Carbide Nanoparticles in Magnetic Heating
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Added by
Juan Manuel Asensio
Publication date
2019
fields
Physics
and research's language is
English
Authors
Juan Asensio
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Heating magnetic nanoparticles with high frequency magnetic fields is a topic of interest for biological applications (magnetic hyperthermia) as well as for heterogeneous catalysis. This study shows why FeC NPs of similar structures and static magnetic properties display radically different heating power (SAR from 0 to 2 kW.g-1). By combining results from Transmission Electron Microscopy (TEM), Dynamic Light Scattering (DLS) and static and time-dependent high-frequency magnetic measurements, we propose a model describing the heating mechanism in FeC nanoparticles. Using, for the first time, time-dependent high-frequency hysteresis loop measurements, it is shown that in the samples displaying the larger heating powers, the hysteresis is strongly time dependent. More precisely, the hysteresis area increases by a factor 10 on a timescale of a few tens of seconds. This effect is directly related to the ability of the nanoparticles to form chains under magnetic excitation, which depends on the presence or not of strong dipolar couplings. These differences are due to different ligand concentrations on the surface of the particles. As a result, this study allows the design of a scalable synthesis of nanomaterials displaying a controllable and reproducible SAR.
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A cornerstone assumption that most literature on discrete time crystals has relied on is that homogeneous Floquet systems generally heat to a featureless infinite temperature state, an expectation that motivated researchers in the field to mostly focus on many-body localized systems. Some works have however shown that the standard diagnostics for time crystallinity apply equally well to clean settings without disorder. This fact raises the question whether an homogeneous discrete time crystal is possible in which the originally expected heating is evaded. Studying both a localized and an homogeneous model with short-range interactions, we clarify this issue showing explicitly the key differences between the two cases. On the one hand, our careful scaling analysis confirms that, in the thermodynamic limit and in contrast to localized discrete time crystals, homogeneous systems indeed heat. On the other hand, we show that, thanks to a mechanism reminiscent of quantum scars, finite-size homogeneous systems can still exhibit very crisp signatures of time crystallinity. A subharmonic response can in fact persist over timescales that are much larger than those set by the integrability-breaking terms, with thermalization possibly occurring only at very large system sizes (e.g., of hundreds of spins). Beyond clarifying the emergence of heating in disorder-free systems, our work casts a spotlight on finite-size homogeneous systems as prime candidates for the experimental implementation of nontrivial out-of-equilibrium physics.
We propose a nonequilibrium variational polaron transformation, based on an ansatz for nonequilibrium steady state (NESS) with an effective temperature, to study quantum heat transport at the nanoscale. By combining the variational polaron transformed master equation with the full counting statistics, we have extended the applicability of the polaron-based framework to study nonequilibrium process beyond the super-Ohmic bath models. Previously, the polaron-based framework for quantum heat transport reduces exactly to the non-interacting blip approximation (NIBA) formalism for Ohmic bath models due to the issue of the infrared divergence associated with the full polaron transformation. The nonequilibrium variational method allows us to appropriately treat the infrared divergence in the low-frequency bath modes and explicitly include cross-bath correlation effects. These improvements provide more accurate calculation of heat current than the NIBA formalism for Ohmic bath models. We illustrate the aforementioned improvements with the nonequilibrium spin-boson model in this work and quantitatively demonstrate the cross-bath correlation, current turnover, and rectification effects in quantum heat transfer.
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.
Every time a chemical reaction occurs, an energy exchange between reactants and environment exists, which is defined as the enthalpy of the reaction. In the last decades, research has resulted in an increasing number of devices at the micro- or nano-scale. Sensors, catalyzers, and energy storage systems are more and more developed as nano-devices which represent the building blocks for commercial macroscopic objects. A general method for the direct evaluation of the energy balance of such systems is not available at present. Calorimetry is a powerful tool to investigate energy exchange, but it usually needs macroscopic sample quantities. Here we report on the development of an original experimental setup able to detect temperature variations as low as 10 mK in a sample of 10 ng using a thermometer device having physical dimensions of 5x5 mm2. The technique has been utilized to measure the enthalpy release during the adsorption process of H2 on a titanium decorated monolayer graphene. The sensitivity of these thermometers is high enough to detect a hydrogen uptake of 10^(-10) moles, corresponding to 0.2 ng, with an enthalpy release of about 23 uJ. The experimental setup allows, in perspective, the scalability to even smaller sizes.
Thermal gradients induce concentration gradients in alkali halide solutions, and the salt migrates towards hot or cold regions depending on the average temperature of the solution. This effect has been interpreted using the heat of transport, which provides a route to rationalize thermophoretic phenomena. Early theories provide estimates of the heat of transport at infinite dilution. These values are used to interpret thermodiffusion (Soret) and thermoelectric (Seebeck) effects. However, accessing heats of transport of individual ions at finite concentration remains an outstanding question both theoretically and experimentally. Here we discuss a computational approach to calculate heats of transport of aqueous solutions at finite concentrations, and apply our method to study lithium chloride solutions at concentrations $>0.5$~M. The heats of transport are significantly different for Li$^+$ and Cl$^-$ ions, unlike what is expected at infinite dilution. We find theoretical evidence for the existence of minima in the Soret coefficient of LiCl, where the magnitude of the heat of transport is maximized. The Seebeck coefficient obtained from the ionic heats of transport varies significantly with temperature and concentration. We identify thermodynamic conditions leading to a maximization of the thermoelectric response of aqueous solutions.
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