We present a detailed description of the implementation of the non-equilibrium Green's function (NEGF) technique on the density-functional-based tight-binding (gDFTB) simulation tool. This approach can be used to compute electronic transport in organic and inorganic molecular-scale devices. The DFTB tight-binding formulation gives an efficient computational tool that is able to handle a large number of atoms. NEGFs are used to compute the electronic density self-consistently with the open-boundary conditions naturally encountered in quantum transport problems and the boundary conditions imposed by the potentials at the contacts. The efficient block-iterative algorithm used to compute the Green's functions is illustrated. The Hartree potential of the density-functional Hamiltonian is obtained by solving the three-dimensional Poisson equation. A scheme to treat geometrically complex boundary conditions is discussed, including the possibility of including multiterminal calculations.
We report on numerical simulations of a zincblende InP surface quantum dot (QD) on buffer. Our model is strictly based on experimental structures, since we extrapolated a three-dimensional dot directly by atomic force microscopy results. Continuum electromechanical, bandstructure and optical calculations are presented for this realistic structure, together with benchmark calculations for a lens-shape QD with the same radius and height of the extrapolated dot. Interesting similarities and differences are shown by comparing the results obtained with the two different structures, leading to the conclusion that the use of a more realistic structure can provide significant improvements in the modeling of QDs fact, the remarkable splitting for the electron p-like levels of the extrapolated dot seems to prove that a realistic experimental structure can reproduce the right symmetry and a correct splitting usually given by atomistic calculations even within the multiband approach. Moreover, the energy levels and the symmetry of the holes are strongly dependent on the shape of the dot. In particular, as far as we know, their wave function symmetries do not seem to resemble to any results previously obtained with simulations of zincblende ideal structures, such as lenses or truncated pyramids. The magnitude of the oscillator strengths is also strongly dependent on the shape of the dot, showing a lower intensity for the extrapolated dot, especially for the transition between the electrons and holes ground state, as a result of a relevant reduction of the wave functions overlap. We also compare an experimental photoluminescence spectrum measured on an homogeneous sample containing about 60 dots with a numerical ensemble average derived from single dot calculations. The broader energy range of the numerical spectrum motivated us to perform further verifications, which have clarified some aspects of the experimental results and helped us to develop a suitable model for the spectrum, by assuming a not equiprobable weight from each dot, a model which is extremely consistent with the experimental data.
We analyze and present applications of a recently proposed empirical tight-binding scheme for investigating the effects of alloy disorder on various electronic and optical properties of semiconductor alloys, such as the band gap variation, the localization of charge carriers, and the optical transitions. The results for a typical antimony-containing III-V alloy, GaAsSb, show that the new scheme greatly improves the accuracy in reproducing the experimental alloy band gaps compared to other widely used schemes. The atomistic nature of the empirical tight-binding approach paired with a reliable parameterization enables more detailed physical insights into the effects of disorder in alloyed materials.
Abstract While graphene grain boundaries (GBs) are well characterized experimentally, their influence on transport properties is less understood. As revealed here, phononic thermal transport is vulnerable to GBs even when they are ultra‐narrow and aligned along the temperature gradient direction. Non‐equilibrium molecular dynamics simulations uncover large reductions in the phononic thermal conductivity ( κ p ) along linear GBs comprising periodically repeating pentagon‐heptagon dislocations. Green's function calculations and spectral energy density analysis indicate that the origin of the κ p reduction is hidden in the periodic GB strain field, which behaves as a reflective diffraction grating with either diffuse or specular phonon reflections, and represents a source of anharmonic phonon–phonon scattering. The non‐monotonic dependence with dislocation density of κ p uncovered here is unaccounted for by the classical Klemens theory. It can help identify GB structures that can best preserve the integrity of the phononic transport.
Abstract Empirical tight-binding (ETB) methods have become a common choice to simulate electronic and transport properties for systems composed of thousands of atoms. However, their performance is profoundly dependent on the way the empirical parameters were fitted, and the found parametrizations often exhibit poor transferability. In order to mitigate some of the the criticalities of this method, we introduce a novel Δ-learning scheme, called MLΔTB. After being trained on a custom data set composed of ab-initio band structures, the framework is able to correlate the local atomistic environment to a correction on the on-site ETB parameters, for each atom in the system. The converged algorithm is applied to simulate the electronic properties of random GaAsSb alloys, and displays remarkable agreement both with experimental and ab-initio test data. Some noteworthy characteristics of MLΔTB include the ability to be trained on few instances, to be applied on 3D supercells of arbitrary size, to be rotationally invariant, and to predict physical properties that are not exhibited by the training set.
We present theoretical and experimental studies of the process of two-wave mixing of broadband radiation in BaTiO3. We show that the energy exchange in such a process can be calculated on the basis of a system of coupled-wave equations in which phase-mismatch diffraction processes are taken into account. Good agreement of the model predictions and measurements performed with a variable-bandwidth Ti:sapphire laser is reported. Reasonable amplification of light with a FWHM spectrum of as much as 10 nm is reported in a standard copropagation scheme; above this value a considerable gain decrease and significant spatial profile changes occur.
This dataset accompanies the publication titled "DFTBephy: A DFTB-based Approach for Electron-Phonon Coupling Calculations". The ZIP file contains results for graphene obtained with DFTBephy for different parametrizations (matsci, mio and 3ob) and one SCC calculation (matsci-scc). The corresponding directories contain the optimized unit-cell (geo_end.gen), the electronic band-structure and phonon dispersion along a band-path (path_el_bandstructure.json and path_ph_bandstructure.json), the (square of the) electron-phonon coupling matrix close to the K-point (el-ph-Nq200-K.hdf5), and the electronic life-times on a k-mesh (relaxation-times-fine.hdf5).
