We investigate the effects of the competition between exchange ($J$) and dipolar ($D$) interactions on the magnetization reversal mechanisms of ferromagnetic nanotubes. Using first atomistic Monte Carlo (MC) simulations for a model with Heisenberg sp
ins on a cylindrical surface, we compute hysteresis loops for a wide range of the $gamma=D/J$ parameter, characterizing the reversal behavior in terms of the cylindrical magnetization components and the vorticity parameter along the tube length. For $gamma$s close to the value for which helical (H) states are stable at zero applied field, we show that the hysteresis loops can occur in four different classes that are combinations of two reversal modes with well-differentiated coercivities with probabilities that depend on the tube length and radius. This variety in the reversal modes is found to be linked to the metastability of the $H$ states during the reversal that induce different paths followed along the energy landscape as the field is changed. We further demonstrate that reversal by either of the two modes can be induced by tailoring the nanotube initial state so that vortices with equal or contrary chirality are formed at the ends, thus achieving low or high coercive fields at will without changing $gamma$. Finally, the results of additional micromagnetic simulations performed on tubes with similar aspect ratio show that dual switching modes and its tailoring can also be observed in tubes with more microscopic dimensions.
A general method for the quantification of dipolar interactions in assemblies of nanoparticles has been developed from a model sample constituted by magnetite nanoparticles of 5 nm in diameter, in powder form with oleic acid as a surfactant so that t
he particles were solely separated from each other through an organic layer of about 1 nm in thickness. This quantification is based on the comparison of the distribution of energy barriers for magnetization reversal obtained from time-dependent relaxation measurements starting from either (i) an almost random orientation of the particles magnetizations or (ii) a collinear arrangement of them prepared by previously field cooling the sample. Experimental results and numerical simulations show that the mean dipolar field acting on each single particle is significantly reduced when particles magnetizations are collinearly aligned. Besides, the intrinsic distribution of the energy barriers of anisotropy for the non-interacting case was evaluated from a reference sample where the same magnetic particles were individually coated with a thick silica shell in order to make dipolar interactions negligible. Interestingly, the results of the numerical simulations account for the relative energy shift of the experimental energy barrier distributions corresponding to the interacting and non-interacting cases, thus supporting the validity of the proposed method for the quantification of dipolar interactions.
Disorder among surface spins largely dominates the magnetic response of ultrafine magnetic particle systems. In this work, we examine time-dependent magnetization in high-quality, monodisperse hollow maghemite nanoparticles with a 14.8 $pm$ 0.5 nm ou
ter diameter and enhanced surface-to-volume ratio. The nanoparticle ensemble exhibits spin-glass-like signatures in dc magnetic aging and memory protocols and ac magnetic susceptibility. The dynamics of the system slows near 50 K, and becomes frozen on experimental time scales below 20 K. Remanence curves indicate the development of magnetic irreversibility concurrent with the freezing of the spin dynamics. A strong exchange-bias effect and its training behavior point to highly frustrated surface spins that rearrange much more slowly than interior spins with bulk coordination. Monte Carlo simulations of a hollow particle reproducing the experimental morphology corroborated strongly disordered surface layers with complex energy landscapes that underlie both glass-like dynamics and magnetic irreversibility. Calculated hysteresis loops reveal that magnetic behavior is not identical at the inner and outer surfaces, with spins at the outer surface layer of the 15 nm hollow particles exhibiting a higher degree of frustration. Our study sheds light on the origin of spin-glass-like phenomena and the role of surface spins in magnetic hollow nanostructures.
In this contribution, we will present a review of our works on the time dependence of magnetization in nanoparticle systems starting from non-interacting systems, presenting a general theoretical framework for the analysis of relaxation curves which
is based on the so-called $svar$ scaling method. We will detail the basics and explain its range of validity, showing also its application in experimental measurements of magnetic relaxation. We will also discuss how it can be applied to determine the energy barrier distributions responsible for the relaxation. Next, we will show how the proposed methodology can be extended to include dipolar interactions between the nanoparticles. A thorough presentation of the method will be presented as exemplified for a 1D chain of interacting spins, with emphasis put on showing the microscopic origin of the observed macroscopic time dependence of the magnetization. Experimental application examples will be given showing that the validity of the method is not limited to 1D case.
Co-based nanostructures ranging from core-shell to hollow nanoparticles were produced by varying the reaction time and the chemical environment during the thermal decomposition of Co2(CO)8. Both structural characterization and kinetic model simulatio
n illustrate that the diffusivities of Co and oxygen determine the growth ratio and the final morphology of the nanoparticles. Exchange coupling between Co and Co-oxide in core/shell nanoparticles induced a shift of field-cooled hysteresis loops that is proportional to the shell thickness, as verified by numerical studies. The increased nanocomplexity when going from core/shell to hollow particles, also leads to the appearance of hysteresis above 300 K due to an enhancement of the surface anisotropy resulting from the additional spin-disordered surfaces.
