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Amilcar Labarta

Publications and source records attributed to Amilcar Labarta.

At least 19 recordsLinked to original sources
arXiv2024

Magnetic nanoparticles: from the nanostructure to the physical properties

Some of the synthesis methods and physical properties of iron-oxide based magnetic nanoparticles such as Fe3-xO4 and CoxFe3-xO4 are reviewed because of their interest in health, environmental applications, and ultra-high-density magnetic recording. Unlike high crystalline quality nanoparticles larger than a few nanometers that show bulk-like magnetic and electronic properties, nanostructures with increasing structural defects yield a progressive worsening of their general performance due to frozen magnetic disorder and local breaking of their crystalline symmetry. Thus, it is shown that single-crystal, monophasic nanoparticles do not exhibit significant surface or finite-size effects, such as spin canting, reduced saturation magnetization, high closure magnetic fields, hysteresis-loop shift or dead magnetic layer features which are mostly associated with crystallographic defective systems. Besides, the key role of the nanoparticle coating, surface anisotropy, and inter-particle interactions are discussed. Finally, the results of some single particle techniques -- magnetic force microscopy, X-ray photoemission electron microscopy, and electron magnetic chiral dichroism -- that allow studying individual nanoparticles down to sub-nanometer resolution with element, valence and magnetic selectivity, are presented. All in all, the intimate, fundamental correlation of the nanostructure (crystalline, chemical, magnetic) to the physical properties of the nanoparticles is ascertained.

cond-mat.mtrl-sci↗
arXiv2024

Geometric frustration in ordered lattices of plasmonic nanoelements

Inspired by geometrically frustrated magnetic systems, we present the optical response of three cases of hexagonal lattices of plasmonic nanoelements. All of them were designed using a metal-insulator-metal configuration to enhance absorption of light, with elements in close proximity to exploit near-field coupling, and with triangular symmetry to induce frustration of the dipolar polarization in the gaps between neighboring structures. Both simulations and experimental results demonstrate that these systems behave as perfect absorbers in the visible and/or the near infrared. Besides, the numerical study of the time evolution shows that they exhibit a relatively extended time response over which the system fluctuates between localized and collective modes. It is of particular interest the echoed excitation of surface lattice resonance modes, which are still present at long times because of the geometric frustration inherent to the triangular lattice. It is worth noting that the excitation of collective modes is also enhanced in other types of arrays where dipolar excitations of the nanoelements are hampered by the symmetry of the array. However, we would like to emphasize that the enhancement in triangular arrays can be significantly larger because of the inherent geometric incompatibility of dipolar excitations and three-fold symmetry axes.

physics.optics↗
arXiv2024

Tunable circular dichroism through absorption in coupled optical modes of twisted triskelia nanostructures

We present a system consisting of two stacked chiral plasmonic nanoelements, so-called triskelia, that exhibits a high degree of circular dichroism. The optical modes arising from the interactions between the two elements are the main responsible for the dichroic signal. Their excitation in the absorption cross section is favored when the circular polarization of the light is opposite to the helicity of the system, so that an intense near-field distribution with 3D character is excited between the two triskelia, which in turn causes the dichroic response. Therefore, the stacking, in itself, provides a simple way to tune both the value of the circular dichroism, up to 60%, and its spectral distribution in the visible and near infrared range. We show how these interaction-driven modes can be controlled by finely tuning the distance and the relative twist angle between the triskelia, yielding maximum values of the dichroism at 20{\deg} and 100{\deg} for left- and right-handed circularly polarized light, respectively. Despite the three-fold symmetry of the elements, these two situations are not completely equivalent since the interplay between the handedness of the stack and the chirality of each single element breaks the symmetry between clockwise and anticlockwise rotation angles around 0{\deg}. This reveals the occurrence of clear helicity-dependent resonances. The proposed structure can be thus finely tuned to tailor the dichroic signal for applications at will, such as highly efficient helicity-sensitive surface spectroscopies or single-photon polarization detectors, among others.

physics.optics↗
arXiv2024

Imaging of Antiferroelectric Dark Modes in an Inverted Plasmonic Lattice

Plasmonic lattice nanostructures are of technological interest because of their capacity to manipulate light below the diffraction limit. Here, we present a detailed study of dark and bright modes in the visible and near-infrared energy regime of an inverted plasmonic honeycomb lattice by a combination of Au+ focused ion beam lithography with nanometric resolution, optical and electron spectroscopy, and finite-difference time-domain simulations. The lattice consists of slits carved in a gold thin film, exhibiting hotspots and a set of bright and dark modes. We proposed that some of the dark modes detected by electron energy-loss spectroscopy are caused by antiferroelectric arrangements of the slit polarizations with two times the size of the hexagonal unit cell. The plasmonic resonances take place within the 0.5_2 eV energy range, indicating that they could be suitable for a synergistic coupling with excitons in two-dimensional transition metal dichalcogenides materials or for designing nanoscale sensing platforms based on near-field enhancement over a metallic surface.

physics.optics↗
arXiv2009

Controlling exchange bias in Co-CoOx nanoparticles by oxygen content

We report on the occurrence of exchange bias on laser-ablated granular thin films composed of Co nanoparticles embedded in amorphous zirconia matrix. The deposition method allows controlling the degree of oxidation of the Co particles by tuning the oxygen pressure at the vacuum chamber (from 2x10^{-5} to 10^{-1} mbar). The nature of the nanoparticles embedded in the nonmagnetic matrix is monitored from metallic, ferromagnetic (FM) Co to antiferromagnetic (AFM) CoOx, with a FM/AFM intermediate regime for which the percentage of the AFM phase can be increased at the expense of the FM phase, leading to the occurrence of exchange bias in particles of about 2 nm in size. For oxygen pressure of about 10-3 mbar the ratio between the FM and AFM phases is optimum with an exchange bias field about 900 Oe at 1.8 K. The mutual exchange coupling between the AFM and FM is also at the origin of the induced exchange anisotropy on the FM leading to high irreversible hysteresis loops, and the blocking of the AFM clusters due to proximity to the FM phase.

cond-mat.mtrl-sci↗
arXiv2009

Magnetic Domains and Surface Effects in Hollow Maghemite Nanoparticles

In the present work, we investigate the magnetic properties of ferrimagnetic and noninteracting maghemite (g-Fe2O3) hollow nanoparticles obtained by the Kirkendall effect. From the experimental characterization of their magnetic behavior, we find that polycrystalline hollow maghemite nanoparticles are characterized by low superparamagnetic-to-ferromagnetic transition temperatures, small magnetic moments, significant coercivities and irreversibility fields, and no magnetic saturation on external magnetic fields up to 5 T. These results are interpreted in terms of the microstructural parameters characterizing the maghemite shells by means of an atomistic Monte Carlo simulation of an individual spherical shell model. The model comprises strongly interacting crystallographic domains arranged in a spherical shell with random orientations and anisotropy axis. The Monte Carlo simulation allows discernment between the influence of the structure polycrystalline and its hollow geometry, while revealing the magnetic domain arrangement in the different temperature regimes.

cond-mat.mtrl-sci↗
arXiv2008

Surface anisotropy broadening of the energy barrier distribution in magnetic nanoparticles

The effect of surface anisotropy on the distribution of energy barriers in magnetic fine particles of nanometer size is discussed within the framework of the $T\ln(t/τ_0)$ scaling approach. The comparison between the distributions of the anisotropy energy of the particle cores, calculated by multiplying the volume distribution by the core anisotropy, and of the total anisotropy energy, deduced by deriving the master curve of the magnetic relaxation with respect to the scaling variable $T\ln(t/τ_0)$, enables the determination of the surface anisotropy as a function of the particle size. We show that the contribution of the particle surface to the total anisotropy energy can be well described by a size--independent value of the surface energy per unit area which permits the superimposition of the distributions corresponding to the particle core and effective anisotropy energies. The method is applied to a ferrofluid composed of non-interacting Fe$_{3-x}$O$_{4}$ particles of 4.9 nm in average size and $x$ about 0.07. Even though the size distribution is quite narrow in this system, a relatively small value of the effective surface anisotropy constant $K_{s}=2.9\times 10^{-2}$ erg cm$^{-2}$ gives rise to a dramatic broadening of the total energy distribution. The reliability of the average value of the effective anisotropy constant, deduced from magnetic relaxation data, is verified by comparing it to that obtained from the analysis of the shift of the ac susceptibility peaks as a function of the frequency.

cond-mat.mtrl-sci↗
arXiv2008

Particle size and cooling field dependence of exchange bias in core/shell magnetic nanoparticles

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.

cond-mat.mtrl-sci↗
arXiv2007

Modelling exchange bias in core/shell nanoparticles

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.

cond-mat.mtrl-sci↗
arXiv2007

Exchange bias phenomenology and models of core/shell nanoparticles

Some of the main experimental observations related to the occurrence of exchange bias in magnetic systems are reviewed, focusing the attention on the peculiar phenomenology associated to nanoparticles with core/shell structure as compared to thin film bilayers. The main open questions posed by the experimental observations are presented and contrasted to existing theories and models for exchange bias formulated up to date. We also present results of simulations based on a simple model of a core/shell nanoparticle in which the values of microscopic parameters such as anisotropy and exchange constants can be tuned in the core, shell and at the interfacial regions, offering new insight on the microscopic origin of the experimental phenomenology. A detailed study of the of the magnetic order of the interfacial spins shows compelling evidence that most of the experimentally observed effects can be qualitatively accounted within the context of this model and allows also to quantify the magnitude of the loop shifts with striking agreement with the macroscopic observed values.

cond-mat.mtrl-sci↗
arXiv2006

Particle growing mechanisms in Ag-ZrO2 and Au-ZrO2 granular films obtained by pulsed laser deposition

Thin films consisting of Ag and Au nanoparticles embedded in amorphous ZrO2 matrix were grown by pulsed laser deposition in a wide range of metal volume concentrations in the dielectric regime (0.08<x(Ag)<0.28 and 0.08<x(Au)<0.52). High resolution transmission electron microscopy (TEM) showed regular distribution of spherical Au and Ag nanoparticles having very sharp interfaces with the amorphous matrix. Mean particle size determined from X-ray diffraction agreed with direct TEM observation. The silver mean diameter increases more abruptly with metal volume content than that corresponding to gold particles prepared under the same conditions. Two mechanisms of particle growing are observed: nucleation and particle coalescence, their relative significance being different in both granular systems, which yields very different values of the percolation threshold (xc(Ag)~0.28 and xc(Au)~0.52).

cond-mat.mtrl-sci↗
arXiv2006

Exchange bias and asymmetric hysteresis loops from a microscopic model of core/shell nanoparticles

We present Monte Carlo simulations of hysteresis loops of a model of a magnetic nanoparticle with a ferromagnetic core and an antiferromegnetic shell with varying values of the core/shell interface exchange coupling which aim to clarify the microscopic origin of exchange bias observed experimentally. We have found loops shifts in the field direction as well as displacements along the magnetization axis that increase in magnitude when increasing the interfacial exchange coupling. Ovelap functions computed from the spin configurations along the loops have been computed to explain the origin and magnitude of these features microscopically.

cond-mat.mtrl-sci↗
arXiv2005

Microscopic origin of exchange bias in core/shell nanoparticles

We report the results of Monte Carlo simulations with the aim to clarify the microscopic origin of exchange bias in the magnetization hysteresis loops of a model of individual core/shell nanoparticles. Increase of the exchange coupling across the core/shell interface leads to an enhancement of exchange bias and to an increasing asymmetry between the two branches of the loops which is due to different reversal mechanisms. A detailed study of the magnetic order of the interfacial spins shows compelling evidence that the existence of a net magnetization due to uncompensated spins at the shell interface is responsible for both phenomena and allows to quantify the loop shifts directly in terms of microscopic parameters with striking agreement with the macroscopic observed values.

cond-mat.mtrl-sci↗
arXiv2005

Monte Carlo simulation study of exchange biased hysteresis loops in nanoparticles

We present the results of Monte Carlo simulations of the magnetic properties of a model for a single nanoparticle consisting in a ferromagnetic core surrounded by an antiferromagnetic shell. The simulations of hysteresis loops after cooling in a magnetic field display exchange bias effects. In order to understand the origin of the loop shifts, we have studied the thermal dependence of the shell and interface magnetizations under field cooling. These results, together with inspection of the snapshots of the configurations attained at low temperature, show the existence of a net magnetization at the interface which is responsible for the bias of the hysteresis loops.

cond-mat.mtrl-sci↗
arXiv2005

From Finite-Size and Surface Effects to Glassy Behaviour in Ferrimagnetic Nanoparticles

This chapter is aimed at studying the anomalous magnetic properties (glassy behaviour) observed at low temperatures in nanoparticles of ferrimagnetic oxides. This topic is discussed both from numerical results and experimental data. Ferrimagnetic fine particles show most of the features of glassy systems due to the random distribution of anisotropy axis, interparticle interactions and surface effects. Experiments have shown that the hysteresis loops display high closure fields with high values of the differential susceptibility. Low magnetisation as compared to bulk, shifted loops after field-cooling, highfield irreversibilities between zero-field and field cooling processes and ageing phenomena in the time-dependence of the magnetisation, are also observed. This phenomenology indicates the existence of some kind of freezing phenomenon arising from a complex hierarchy of the energy levels, whose origin is currently under discussion. Two models have been proposed to account for it: i) the existence of a spin-glass state at the surface of the particle which is coupled to the particle core through an exchange field; and ii) the collective behaviour induced by interparticle interactions. In real systems, both contributions simultaneously occur, being difficult to distinguish their effects. In contrast, numerical simulations allow us to build a model just containing the essential ingredients to study solely one of two phenomena.

cond-mat.mtrl-sci↗
arXiv2004

Influence of surface anisotropy on the hysteresis of magnetic nanoparticles

We present the results of Monte Carlo simulations of the magnetic properties of individual spherical nanoparticles with the aim to explain the role played by surface anisotropy on their low temperature magnetization processes. Phase diagrams for the equilibrium configurations have been obtained, showing a change from quasi-uniform magnetization state to a state with hedgehog-like structures at the surface as $k_S$ increases. Through the simulated hysteresis loops and the analysis of spin configurations along them, we have identified a change in the magnetization reversal mechanism from quasi-uniform rotation at low $k_S$ values, to a non-uniform switching process at high $k_S$. Results for the dependence of the coercive field and remanence on $k_S$ and particle size are also reported.

cond-mat.mtrl-sci↗
arXiv2004

Magnetic relaxation in a model of interacting nanoparticles in terms of microscopic energy barriers

Monte Carlo simulations are used to study the magnetic relaxation of a system of single domain particles with dipolar interactions modeled by a chain of Heisenberg classical spins. We show that the so-called $T\ln(t/τ_0)$ method can be extended to interacting systems and how, from the computed master relaxation curves, the effective energy barrier distributions responsible for the relaxation can be obtained. A transition from a quasi-logarithmic to power-law behavior of the relaxation as the interaction strength is in-creased is found. By direct computation of the effective energy barriers of the system, we show that this is due to the appearance of an increasing number of small energy barriers caused by the reduction of the anisotropy energy barriers as the local dipolar fields increase.

cond-mat.mtrl-sci↗