Searcharxiv⌕ Search

arXiv subjects

Xavier Batlle

Publications and source records attributed to Xavier Batlle.

At least 19 recordsLinked to original sources
arXiv2025

Single-particle detection of a semiconductor-to-metal transition by scanning dielectric microscopy

Hybrid nanostructures that combine semiconducting and metallic components offer great potential for photothermal therapy, optoelectronics, and sensing, by integrating tunable optical properties with enhanced light absorption and charge transport. Boosting the integrated performance of these hybrid systems demands techniques capable of probing local variations of the physical properties inaccessible to bulk analysis. Here, we report the single-particle dielectric characterization of hybrid, semiconducting bismuth sulfide (Bi$_2$S$_3$) nanorods (NR) decorated with metallic Au nanoparticles (NP), employing scanning dielectric microscopy, which uses electrostatic force microscopy in combination with finite-element numerical simulations. We reveal a pronounced enhancement in the local dielectric response of Bi$_2$S$_3$ upon Au decoration, attributed to interfacial polarization and electron transfer from Au to the Bi$_2$S$_3$ matrix, thus suggesting a semiconductor-to-metal-like transition at the single-particle level. Numerical simulations show that the response is dominated by the vertical component of the permittivity and that the decorating metallic Au NP produce only moderate shielding of the semiconductor Bi$_2$S$_3$ NR core, indicating that the large increase in the dielectric response originates primarily from intrinsic modifications within the NR. Overall, these findings provide direct insight into structure--property relationships at the single-particle level, supporting the rational design of advanced hybrid nanostructures with tailored electronic functionalities.

physics.chem-ph↗
arXiv2025

Dichroism of coupled multipolar plasmonic modes in twisted triskelion stacks

We present a systematic investigation of the optical response to circularly polarized illumination in twisted stacked plasmonic nanostructures. The system consissts in two identical, parallel gold triskelia centrally aligned and rotated at a central angle relative to each other. Sample fabrication was acomplished through a double electron beam lithograpy process. This stack holds two plasmonic modes of multipolar character in the near-infrared range, showing a strong dependence of their excitation intensities on the handedness of the circularly polarized incident light. This translates in a large circular dicrhoism which can be modulated by adjusting the twist angle of the stack. Fourier-transform infrared spectroscopy and numerical simulations were employed to characterize the spectral features of the modes. Remarkable, in contrast to previous results in other stacked nanostructures, the system's response exhibits a behavious analogous to that of two interacting dipoles only at small angles. As the angle approaches 15 degrees, where the maximum dichroism is observed, more complex modes of the stack emerge. These modes evolve towards two in-phase multipolar excitations of the two triskelia as the angle increases uo to 60 degrees. Finally, simulations for a triangular array of such stacked elements show a sharp mode arising from the hybridization of a surface lattice resonance with the low-energy mode of the stack.

physics.optics↗
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↗
arXiv2021

Deconvolution of phonon scattering by ferroelectric domain walls and point defects in a PbTiO3 thin film deposited in a composition-spread geometry

We present a detailed analysis of the temperature dependence of the thermal conductivity of a ferroelectric PbTiO3 thin film deposited in a composition-spread geometry enabling a continuous range of compositions from ~25% titanium-deficient to ~20% titanium-rich to be studied. By fitting the experimental results to the Debye model we deconvolve and quantify the two main phonon scattering sources in the system: ferroelectric domain walls (DWs) and point defects. Our results prove that ferroelectric DWs are the main agent limiting the thermal conductivity in this system, not only in the stoichiometric region of the thin film ([Pb]/[Ti]~1), but also when the concentration of cation point defects is significant (up to ~15%). Hence, DWs in ferroelectric materials are a source of phonon scattering at least as effective as point defects. Our results demonstrate the viability and effectiveness of using reconfigurable DWs to control the thermal conductivity in solid-state devices.

cond-mat.mtrl-sci↗
arXiv2015

Quantification of dipolar interactions in Fe$_{3-x}$O$_4$ nanoparticles

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 the 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.

cond-mat.mtrl-sci↗
arXiv2010

Magnetic nanoparticles with bulk-like properties

The magnetic behavior of $Fe_{3-x}O_4$ nanoparticles synthesized either by high-temperature decomposition of an organic iron precursor or low-temperature co-precipitation in aqueous conditions, is compared. Transmission electron microscopy, X-ray absorption spectroscopy, X-ray magnetic circular dichroism and magnetization measurements show that nanoparticles synthesized by thermal decomposition display high crystal quality and bulk-like magnetic and electronic properties, while nanoparticles synthesized by co-precipitation show much poorer crystallinity and particle-like phenomenology, including reduced magnetization, high closure fields and shifted hysteresis loops. The key role of the crystal quality is thus suggested since particle-like behavior for particles larger than about 5 nm is only observed when they are structurally defective. These conclusions are supported by Monte Carlo simulations. It is also shown that thermal decomposition is capable of producing nanoparticles that, after further stabilization in physiological conditions, are suitable for biomedical applications such as magnetic resonance imaging or bio-distribution studies.

cond-mat.mtrl-sci↗
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↗
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↗
arXiv2006

Asymmetric Reversal in Inhomogeneous Magnetic Heterostructures

Asymmetric magnetization reversal is an unusual phenomenon in antiferromagnet / ferromagnet (AF/FM) exchange biased bilayers. We investigated this phenomenon in a simple model system experimentally and by simulation assuming inhomogeneously distributed interfacial AF moments. The results suggest that the observed asymmetry originates from the intrinsic broken symmetry of the system, which results in local incomplete domain walls parallel to the interface in reversal to negative saturation of the FM. Magneto-optic Kerr effect unambiguously confirms such an asymmetric reversal and a depth-dependent FM domain wall in accord with the magnetometry and simulations.

cond-mat.mtrl-sci↗