arXiv subjects

Fábio D. A. Aarão Reis

Publications and source records attributed to Fábio D. A. Aarão Reis.

9 recordsLinked to original sources

arXiv2026

Modeling electrodeposition of thin films with compact, dendritic, and random morphologies

We summarize previously published computer simulation studies of a metal electrodeposition model that considers diffusive cation flux, a fast reaction in contact with the electrode or with the growing deposit, and adsorbed atom diffusion in finite time windows. Simulations with various parameters show compact, fractal, dendritic deposits, and dynamic transitions between different morphologies during the growth of individual samples. The dendritic shapes are characterized by hierarchical organizations in which branches of a given order reproduce the shape and crystalline orientation of the branches of the previous order, in contrast to the random branching of the fractal deposits formed by DLA and related models. The simulations show dendrites with maple leaf shape in SC lattices, pine tree shape in FCC lattices, and flower-like shape in HCP lattices, with surfaces predominantly oriented in the lowest-energy configurations of each lattice. Simulations with nucleation restricted to a nanoscale seed show the initial formation of faceted particles followed by dendrite formation, in agreement with silver electrodeposition on substrates patterned with gold nanoparticles. A quantitative application to faceted and dendritic silver obtained in the same experiment provides values of the model parameters which are consistent with the characteristic widths of these structures being of the same order of magnitude of the diffusion lengths of atoms on (111) and (001) surfaces. Using an extended model for iron electrodeposition on Si(100), the simulations qualitatively reproduce the initial formation of multilayer islands, small oscillations of the roughness of a polycrystalline compact film after island coalescence, and instability development. Possible directions for applying this modeling to the electrodeposition of other materials are suggested.

cond-mat.mtrl-sci↗

arXiv2026

Non-monotonic roughness evolution in film growth on weakly interacting substrates

Thin film deposition on weakly interacting substrates exhibits a unique growth mode characterized by initially strong island formation and rapidly increasing roughness, which reaches a maximum and subsequently decreases as the film returns to a smooth morphology. Here we show this rough-to-smooth growth mode experimentally for two molecular systems with substantially different geometries, namely, the effectively spherical buckminsterfullerene (C$_{60}$) and the disk-like 1,4,5,8,9,11-hexaazatriphenylenehexacarbonitrile (HATCN). This growth mode is explained by a geometrical model that captures the basic mechanisms of multilayer island growth, island coalescence, and formation of a continuous film. Additionally, kinetic Monte Carlo simulations with minimal ingredients demonstrate that this mode generally occurs for weakly interacting substrates, providing quantitative estimates of parameters that characterize adsorbate-adsorbate and adsorbate-substrate interactions. Both the model and simulations accurately describe the experimental data and highlight the generic nature of the phenomenon, independently of the details of the interactions and the molecular flux, which opens up a path for controlling nanoscale film roughness.

cond-mat.mtrl-sci↗

arXiv2024

Island formation in heteroepitaxial growth

Island formation in strain-free heteroepitaxial deposition of thin films is analyzed using kinetic Monte Carlo simulations of two minimal lattice models and scaling approaches. The transition from layer-by-layer (LBL) to island (ISL) growth is driven by a weaker binding strength of the substrate which, in the kinetic model, is equivalent to an increased diffusivity of particles on the substrate compared to particles on the film. The LBL-ISL transition region is characterized by particle fluxes between layers 1 and 2 significantly exceeding the net flux between them, which sets a quasi-equilibrium condition. Deposition on top of monolayer islands weakly contributes to second layer nucleation, in contrast with the homoepitaxial growth case. A thermodynamic approach for compact islands with one or two layers predicts the minimum size in which the second layer is stable. When this is linked to scaling expressions for submonolayer island deposition, the dependence of the ISL-LBL transition point on the kinetic parameters qualitatively matches the simulation results, with quantitative agreement in some parameter ranges. The transition occurs in the equilibrium regime of partial wetting and the convergence of the transition point upon reducing the deposition rate is very slow and practically unattainable in experiments.

cond-mat.soft↗

arXiv2024

Effective medium theory for the electrical conductance of random resistor networks which mimic crack-template-based transparent conductive films

We studied random resistor networks produced with regular structure and random distribution of edge conductances. These networks are intended to mimic crack-template-based transparent conductive films as well some random networks produced using nano-imprinting technology. Applying an effective medium theory, we found out that the electrical conductance of such networks is $\approx 0.5852 \sqrt{n_E}$, where $n_E$ is the number density of conductive edges. This dependence is in agreement with numerical calculations in Voronoi networks, although the effective conductances are approximately 15\% larger.

cond-mat.dis-nn↗

arXiv2021

Roughness and Correlations in the Transition from Island to Film Growth: Simulations and Application to CdTe Deposition

Using kinetic Monte Carlo simulations, we develop a framework to relate morphological properties and microscopic dynamics during island growth, coalescence, and initial formation of continuous heteroepitaxial films. The average island width is controlled by adatom mobility on the substrate. Subsequent evolution strongly depends on the Ehrlich-Schwöebel energy barrier $E_{ES}$ of the deposited material. As $E_{ES}$ decreases, islands becomes taller and their coalescence is delayed. For small islands and large $E_{ES}$, the global roughness increases as $W\sim{\text{thickness}}^{1/2}$ and the local roughness increases at short scales (apparent anomalous scaling) before and after island coalescence. If the islands are wide, $W$ may have a plateau for large $E_{ES}$ and has a maximum for small $E_{ES}$ when the islands coalesce. This framework is applied to atomic-force microscopy data of the initial stages of CdTe deposition on Kapton: a maximum of $W$ during island coalescence indicates negligible ES barrier, consistently with scaling properties of much thicker films, and the diffusion coefficient ${10}^{-7}{\text{--}}{10}^{-5}{\text{cm}}^2/{\text s}$ on the Kapton surface at $150\,^{\circ}\mathrm{C}$ is estimated. Applications of the framework to other materials are suggested, in which the expected roles of ES barriers are highlighted.

cond-mat.mtrl-sci↗

arXiv2021

Time increasing rates of infiltration and reaction in porous media at the percolation thresholds

The infiltration of a solute in a fractal porous medium is usually anomalous, but chemical reactions of the solute and that material may increase the porosity and affect the evolution of the infiltration. We study this problem in two- and three-dimensional lattices with randomly distributed porous sites at the critical percolation thresholds and with a border in contact with a reservoir of an aggressive solute. The solute infiltrates that medium by diffusion and the reactions with the impermeable sites produce new porous sites with a probability $r$, which is proportional to the ratio of reaction and diffusion rates at the scale of a lattice site. Numerical simulations for $r\ll1$ show initial subdiffusive scaling and long time Fickean scaling of the infiltrated volumes or areas, but with an intermediate regime with time increasing rates of infiltration and reaction. The anomalous exponent of the initial regime agrees with a relation previously applied to infinitely ramified fractals. We develop a scaling approach that explains the subsequent time increase of the infiltration rate, the dependence of this rate on $r$, and the crossover to the Fickean regime. The exponents of the scaling relations depend on the fractal dimensions of the critical percolation clusters and on the dimensions of random walks in those clusters. The time increase of the reaction rate is also justified by that reasoning. As $r$ decreases, there is an increase in the number of time decades of the intermediate regime, which suggests that the time increasing rates are more likely to be observed is slowly reacting systems.

cond-mat.stat-mech↗

arXiv2020

Statistics of adatom diffusion in a model of thin film growth

We study the statistics of the number of executed hops of adatoms at the surface of films grown with the Clarke-Vvedensky (CV) model in simple cubic lattices. The distributions of this number, $N$, are determined in films with average thicknesses close to $50$ and $100$ monolayers for a broad range of values of the diffusion-to-deposition ratio $R$ and of the probability $ε$ that lowers the diffusion coefficient for each lateral neighbor. The mobility of subsurface atoms and the energy barriers for crossing step edges are neglected. Simulations show that the adatoms execute uncorrelated diffusion during the time in which they move on the film surface. In a low temperature regime, typically with $Rε\lesssim 1$, the attachment to lateral neighbors is almost irreversible, the average number of hops scales as $\langle N\rangle \sim R^{0.38\pm 0.01}$, and the distribution of that number decays approximately as $\exp\left[-\left({N/\langle N\rangle}\right)^{0.80\pm 0.07}\right]$. Similar decay is observed in simulations of random walks in a plane with randomly distributed absorbing traps and the estimated relation between $\langle N\rangle$ and the density of terrace steps is similar to that observed in the trapping problem, which provides a conceptual explanation of that regime. As the temperature increases, $\langle N\rangle$ crosses over to another regime when $Rε^{3.0\pm 0.3}\sim 1$, which indicates high mobility of all adatoms at terrace borders. The distributions $P\left( N\right)$ change to simple exponential decays, due to the constant probability for an adatom to become immobile after being covered by a new deposited layer. At higher temperatures, the surfaces become very smooth and $\langle N\rangle \sim Rε^{1.85\pm 0.15}$, which is explained by an analogy with submonolayer growth.

cond-mat.stat-mech↗

arXiv2020

Domain formation in the deposition of thin films of two-component mixtures

We perform a kinetic Monte Carlo simulation study of a model of thin film deposition of a two-component mixture in which the activation energy for diffusion of an adatom is additive over its nearest neighbors and in which the interactions between adatoms of the same species are stronger than those between adatoms of different species. The film morphology is investigated for broad ranges of values of the ratios between terrace diffusivity and atomic flux, of the probabilities of detachment from lateral neighbors, and of probabilities of crossing terrace edges. First, we consider a symmetric case in which the interactions of adatoms of the same species are the same for the two components. For low and intermediate temperatures, we show the formation of narrow domains, whose widths are $3$-$30$ lattice constants, which meander in the layers parallel to the substrate, and are connected through very long distances. The domain width depends on the diffusivity-flux ratio of the same species, but it is weakly affected by interactions of different species, so rough estimates of that width can be obtained by using tabulated properties of films with a single component. At high temperatures, the separation of domains is enhanced, but their long distance connectivity is lost, which shows that the formation of the long meandering domains is restricted to a certain range of temperature and flux. Similar morphological features are obtained when the intra-species interactions are different and the adatom diffusion coefficients on terraces of the same species differ up to two orders of magnitude. An approximate scaling relation for the domain width is obtained, but the species with the largest mobility constrains the temperature range in which the long connected domains are found.

cond-mat.mtrl-sci↗

arXiv2020

Thin film growth models with long surface diffusion lengths

In limited mobility (LM) models of thin film deposition, the final position of each atom or molecule is chosen according to a set of stochastic rules before the incidence of another atom or molecule. Here we investigate the possibility of a LM model to reproduce features of a more realistic approach that represents the interplay of collective adatom diffusion and the external flux. In the LM model introduced here, each adatom may execute $G$ hops to neighboring columns of the deposit, but a hop attempt from a site with $n$ lateral neighbors has probability $P^n$, with $P<1$. These rules resemble those of the Clarke-Vvedensky (CV) model without energy barriers at step edges, whose main parameters are the diffusion-to-deposition ratio $R$ on terraces and the detachment probability $ε$ per lateral neighbor. At short times, the roughness of the LM model can be written in terms of a scaling function of $G$ and $P$ and the growth exponent is consistent with the Villain-Lai-Das Sarma universality class. The evolution of the surface roughness and of the autocorrelation function of the CV model is reproduced with reasonable accuracy by the LM model with suitable choices of parameters. The increase of the parameters $G$ and $R$ of those models produces smoother film surfaces, while the increase of $P$ and $ε$ smoothen the terrace boundaries at short lengthscales. However, the detachment probabilities of the two models have very different effects on the surface roughness: in the LM model, for fixed $G$, the surface roughness increases as $P$ increases; in the CV model, the surface smoothens as $ε$ increases, for fixed $R$. This result is related to the non-Markovian nature of the LM model, since the diffusivity of an adatom depends on its history at the film surface and may be severely reduced after a detachment from a terrace step.

cond-mat.stat-mech↗