arXiv subjects

Juan J. Meléndez

Publications and source records attributed to Juan J. Meléndez.

10 recordsLinked to original sources

arXiv2026

Optical properties of single-crystal As2Se3 from first principles

Crystalline As2Se3 is a promising layered chalcogenide for mid-infrared photonics and optoelectronic applications, yet its fundamental electronic and optical properties remain debated. This paper combines density functional theory with G0W0 quasiparticle corrections and Bethe-Salpeter equation (BSE) calculations to deliver a robust description of its band structure and optical response. The G0W0 results reveal an indirect band gap of 2.31 eV with nearly degenerate direct transitions at Gamma, while the BSE spectra exhibit strong polarization-dependent anisotropy and pronounced excitonic effects. Several bound excitons are identified near the absorption onset, clarifying the role of electron-hole interactions and resolving previous controversies regarding the nature of the optical gap and the contribution of lone-pair states. This work provides a unified and quantitatively accurate picture of As2Se3, reinforcing its potential for next-generation infrared and anisotropic photonic devices.

cond-mat.mtrl-sci↗

arXiv2026

Exponents and front fluctuations in the quenched Kardar-Parisi-Zhang universality class of one- and two- dimensional interfaces

We have simulated an automaton version of the quenched Kardar-Parisi-Zhang (qKPZ) equation in one and two dimensions in order to study the scaling properties of the interface at the depinning transition. Specifically, the $α$, $β$, $θ$, and $δ$ critical exponents characterizing the surface kinetic roughening and depinning behaviors have been directly computed from the simulations. In addition, by studying the height-difference correlation function in real space, we have also been able to directly compute the dynamic correlation length and its associated dynamic critical exponent $z$. The full sets of scaling exponents are largely compatible with those of the Directed Percolation Depinning universality class for one and two dimensional interfaces. Furthermore, we have computed numerically the probability density function (PDF) of the front fluctuations in the growth regime, finding its asymptotic form in one and two dimensions. While the PDF features strongly non-Gaussian skewness and kurtosis values, it also differs from the PDF of the KPZ equation with time-dependent noise for physical substrate dimensions, both in the central part and at the tails of the distribution.

cond-mat.stat-mech↗

arXiv2024

Polarization-dependent excitons and plasmon activity in nodal-line semimetal ZrSiS

The optical properties of bulk ZrSiS nodal-line semimetal are theoretically studied within a many-body formalism. The G0W0 bands are similar to those calculated within the density functional theory, except near the Γ point; in particular, no significant differences are found around the Fermi energy. On the other hand, the solution of the Bethe-Salpeter equation reveals a significant excitonic activity, mostly as dark excitons which appear in a wide energy range. Bright excitons, on the contrary, are less numerous, but their location and intensity depend greatly on the polarization of the incident electric field, as the absorption coefficient itself does. The binding energy of these excitons correlate well with their spatial distribution functions. In any case, a good agreement with available experimental data for absorption-reflection is achieved. Finally, the possible activation of plasma oscillations at low energies is discarded, because these are damped by producing electron-hole pairs, more importantly for q along the Γ-M path.

cond-mat.mes-hall↗

arXiv2024

Role of Inorganic Cations in the Excitonic Properties of Lead Halide Perovskites

We theoretically investigate lead iodide perovskites of general formula APbI$_3$ for a series of metallic cations (namely Cs$^+$, Rb$^+$, K$^+$, Na$^+$ and Li$^+$) by means of the density functional theory, GW method and Bethe-Salpeter equation including spin-orbit coupling. We demonstrate that the low-energy edges (up to 1.3 eV) of the absorption spectra are dominated by weakly bound excitons, with binding energies $E_b$ $\sim$ 30-80~meV, and the corresponding intensities grow as metallic %A$^+$ cations become lighter. The middle parts of the spectra (1.8-2.4 eV), on the other hand, contain optical dipole transitions comprising more strongly bound excitons ($E_b$ $\sim$ 150-200~meV) located at PbI$_3$. These parts of the spectra correspond to the optical-gain wavelengths which are experimentally achieved in optically-pumped perovskite lasers. Finally, the higher energy parts, from about 2.8~eV (LiPbI$_3$) to 4.3 eV (CsPbI$_3$), contain optical transitions with very strongly bound excitons ($E_b$ $\sim$ 220-290~meV) located at the halide atoms and the empty states of the metallic cations.

cond-mat.mtrl-sci↗

arXiv2024

Exploring epitaxial structures for electrically pumped perovskite lasers: a study of CsPb(Br,I)$_3$ based on the \textit{ab initio} Bethe-Salpeter equation

Halide perovskites are widely used as components of electronic and optoelectronic devices such as solar cells, light-emitting diodes (LEDs), optically pumped lasers, field-effect transistors, photodetectors, and $γ$-detectors. Despite this wide range of applications, the construction of an electrically pumped perovskite laser remains challenging. In this paper, we numerically justify that mixing two perovskite compounds with different halide elements can lead to optical properties suitable for electrical pumping. As a reference, the chosen model material was CsPbBr$_3$, whose performance as a part of lasers has been widely recognised, with some Br atoms substituted by I at specific sites. In particular, a strong enhancement of the low-energy absorption peaks has been obtained using the \textit{ab initio} Bethe-Salpeter equation. Based on these results, we propose specific architectures of ordered doping that could be realised by epitaxial growth. Efficient light emission from the bottom of the conduction band is expected.

cond-mat.mtrl-sci↗

arXiv2020

Investigating charge carrier scattering processes in anisotropic semiconductors through first-principles calculations: The case of p-type SnSe

Efficient ab initio computational methods for the calculation of thermoelectric transport properties of materials are of great avail for energy harvesting technologies. The BoltzTraP code has been largely used to efficiently calculate thermoelectric coefficients. However, its current version that is publicly available is based only on the constant relaxation time (RT) approximation, which usually does not hold for real materials. Here, we extended the implementation of the BoltzTraP code by incorporating realistic k-dependent RT models of the temperature dependence of the main scattering processes, namely, screened polar and nonpolar scattering by optical phonons, scattering by acoustic phonons, and scattering by ionized impurities with screening. Our RT models are based on a smooth Fourier interpolation of Kohn-Sham eigenvalues and its derivatives, taking into account non-parabolicity (beyond the parabolic or Kane models), degeneracy and multiplicity of the energy bands on the same footing, within very low computational cost. In order to test our methodology, we calculated the anisotropic thermoelectric transport properties of low temperature phase (Pnma) of intrinsic p-type and hole-doped tin selenide (SnSe). Our results are in quantitative agreement with experimental data, regarding the evolution of the anisotropic thermoelectric coefficients with both temperature and chemical potential. Hence, from this picture, we also obtained the evolution and understanding of the main scattering processes of the overall thermoelectric transport in p-type SnSe.

cond-mat.mtrl-sci↗

arXiv2017

Ultralow and Anisotropic Thermal Conductivity in Semiconductor As2Se3

An ultralow lattice thermal conductivity of 0.14 W$\cdot$ m$^{-1} \cdot$ K$^{-1}$ along the $\vec b$ axis of As$_2$Se$_3$ single crystals was obtained at 300 K by first-principles calculations involving the density functional theory and the resolution of the Boltzmann transport equation. This ultralow lattice thermal conductivity arises from the combination of two mechanisms: 1) a cascade-like fall of the low-lying optical modes, which results in avoided crossings of these with the acoustic modes, low sound velocities and increased scattering rates of the acoustic phonons; and 2) the repulsion between the lone-pair electrons of the As cations and the valence $p$ orbitals of the Se anions, which leads to an increase in the anharmonicity of the bonds. The physical origins of these mechanisms lie on the nature of the chemical bonding in the material and its strong anisotropy. These results, whose validity has been addressed by comparison with SnSe, for which excellent agreement between the theoretical predictions and the experiments is achieved, point out that As$_2$Se$_3$ could exhibit improved thermoelectric properties.

cond-mat.mtrl-sci↗

arXiv2016

$zT$-factor enhancement in SnSe: predictions from first principles calculations

The electronic structure and thermoelectric properties of SnSe are studied by first-principles methods. The inclusion of van der Waals dispersive corrections improves the agreement of structural parameters with experiments. The bands structure and projected density of states justify the macroscopic anisotropy exhibited by this system. An original methodology is used to estimate the chemical potential and the relaxation time for the electrical and thermal conductivities. Following this methodology, the Seebeck coefficient and thermal conductivity for single crystals and polycrystals are described in good agreement with experimental data. As for the electrical conductivity, values calculated with a temperature-dependent relaxation time compare well with available measurements, especially for single crystals, polycrystals are better described by a constant relaxation time. Finally, the figure of merit of SnSe single crystals and polycrystals is calculated. It is found to exhibit a maximum for some "ideal" carrier concentration, and might be noticeably enhanced by using carrier concentrations higher than the experimental ones. From these findings, possible strategies to increase the figure of merit in practise are suggested.

cond-mat.mtrl-sci↗

arXiv2016

Numerical matrix method for quantum periodic potentials

A numerical matrix methodology is applied to quantum problems with periodic potentials. The procedure consists essentially in replacing the true potential by an alternative one, restricted by an infinite square well, and in expressing the wave functions as finite superpositions of eigenfunctions of the infinite well. A matrix eigenvalue equation then yields the energy levels of the periodic potential within an acceptable accuracy. The methodology has been successfully used to deal with problems based on the well-known Kronig-Penney (KP) model. Besides the original model, these problems are a dimerized KP solid, a KP solid containing a surface, and a KP solid under an external field. A short list of additional problems that can be solved with this procedure is presented.

quant-ph↗

arXiv2015

In2O3 doped with hydrogen: electronic structure and optical properties from the pseudopotential Self-Interaction Corrected Density Functional Theory and the Random Phase Approximation

We discuss the applicability of the pseudopotential-like self-interaction correction (pSIC) to the study of defect energetics and electronic structure of In2O3. Our results predict that substitutional (at oxygen sites) and interstitial (at antibonding positions) hydrogen, as well as oxygen vacancies with charges +1 and +2, are stable configurations of defects in cubic In2O3; the former form shallow levels (only as substitutional defects), whereas the latter form deep levels. The band structure calculated with the pSIC shows an excellent agreement with experimental data. In particular, the gap for defect-free In2O3 is 2.85 eV, which compares fairly with the experimental range 2.3-2.9 eV. The pSIC results also point to a change from indirect to direct gaps depending on doping. In relation to the optical properties, obtained within the random phase approximation, it is shown that they are mostly affected by the presence of oxygen vacancies.

cond-mat.mtrl-sci↗