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Ivo Souza

Publications and source records attributed to Ivo Souza.

66 records · Page 4Linked to original sources
arXiv2006

Nonlinear optics of III-V semiconductors in the terahertz regime: an ab-initio study

We compute from first principles the infrared dispersion of the nonlinear susceptibility $χ^{(2)}$ in zincblende semiconductors. At terahertz frequencies the nonlinear susceptibility depends not only on the purely electronic response $χ^{(2)}_{\infty}$, but also on three other parameters $C_1$, $C_2$ and $C_3$ describing the contributions from ionic motion. They relate to the TO Raman polarizability, the second-order displacement-induced dielectric polarization, and the third-order lattice potential. Contrary to previous theory, we find that mechanical anharmonicity ($C_3$) dominates over electrical anharmonicity ($C_2$), which is consistent with recent experiments on GaAs. We predict that the sharp minimum in the intensity of second-harmonic generation recently observed for GaAs between $ω_{\rm TO}/2$ and $ω_{\rm TO}$ does not occur for several other III-V compounds.

cond-mat.mtrl-sci↗
arXiv2006

Ab initio calculation of the anomalous Hall conductivity by Wannier interpolation

The intrinsic anomalous Hall effect in ferromagnets depends on subtle spin-orbit-induced effects in the electronic structure, and recent ab-initio studies found that it was necessary to sample the Brillouin zone at millions of k-points to converge the calculation. We present an efficient first-principles approach for computing the anomalous Hall conductivity. We start out by performing a conventional electronic-structure calculation including spin-orbit coupling on a uniform and relatively coarse k-point mesh. From the resulting Bloch states, maximally-localized Wannier functions are constructed which reproduce the ab-initio states up to the Fermi level. The Hamiltonian and position-operator matrix elements, needed to represent the energy bands and Berry curvatures, are then set up between the Wannier orbitals. This completes the first stage of the calculation, whereby the low-energy ab-initio problem is transformed into an effective tight-binding form. The second stage only involves Fourier transforms and unitary transformations of the small matrices set up in the first stage. With these inexpensive operations, the quantities of interest are interpolated onto a dense k-point mesh and used to evaluate the anomalous Hall conductivity as a Brillouin zone integral. The present scheme, which also avoids the cumbersome summation over all unoccupied states in the Kubo formula, is applied to bcc Fe, giving excellent agreement with conventional, less efficient first-principles calculations. Remarkably, we find that more than 99% of the effect can be recovered by keeping a set of terms depending only on the Hamiltonian matrix elements, not on matrix elements of the position operator.

cond-mat.mtrl-sci↗
arXiv2003

Dynamics of Berry-phase polarization in time-dependent electric fields

We consider the flow of polarization current J(t)=dP/dt produced by a homogeneous electric field E(t) or by rapidly varying some other parameter in the Hamiltonian of a solid. For an initially insulating system and a collisionless time evolution, the dynamic polarization P(t) is given by a nonadiabatic version of the King-Smith--Vanderbilt geometric-phase formula. This leads to a computationally convenient form for the Schroedinger equation where the electric field is described by a linear scalar potential handled on a discrete mesh in reciprocal space. Stationary solutions in sufficiently weak static fields are local minima of the energy functional of Nunes and Gonze. Such solutions only exist below a critical field that depends inversely on the density of k points. For higher fields they become long-lived resonances, which can be accessed dynamically by gradually increasing E. As an illustration the dielectric function in the presence of a dc bias field is computed for a tight-binding model from the polarization response to a step-function discontinuity in E(t), displaying the Franz-Keldysh effect.

cond-mat.mtrl-sci↗
arXiv2003

Ab-initio transport properties of nanostructures from maximally-localized Wannier functions

We present a comprehensive first-principles study of the ballistic transport properties of low dimensional nanostructures such as linear chains of atoms (Al, C) and carbon nanotubes in presence of defects. A novel approach is introduced where quantum conductance is computed from the combination of accurate plane-wave electronic structure calculations, the evaluation of the corresponding maximally-localized Wannier functions, and the calculation of transport properties by a real-space Green's function method based on the Landauer formalism. This approach is computationally very efficient, can be straightforwardly implemented as a post-processing step in a standard electronic-structure calculation, and allows to directly link the electronic transport properties of a device to the nature of the chemical bonds, providing insight onto the mechanisms that govern electron flow at the nanoscale.

cond-mat.mes-hall↗
arXiv2003

Current-Density Functional Theory of the Response of Solids

The response of an extended periodic system to a homogeneous field (of wave-vector $q=0$) cannot be obtained from a $q=0$ time-dependent density functional theory (TDDFT) calculation, because the Runge-Gross theorem does not apply. Time-dependent {\em current}-density functional theory is needed and demonstrates that one key ingredient missing from TDDFT is the macroscopic current. In the low-frequency limit, in certain cases, density polarization functional theory is recovered and a formally exact expression for the polarization functional is given.

cond-mat.mtrl-sci↗
arXiv2002

A First-Principles Approach to Insulators in Finite Electric Fields

We describe a method for computing the response of an insulator to a static, homogeneous electric field. It consists of iteratively minimizing an electric enthalpy functional expressed in terms of occupied Bloch-like states on a uniform grid of k points. The functional has equivalent local minima below a critical field E_c that depends inversely on the density of k points; the disappearance of the minima at E_c signals the onset of Zener breakdown. We illustrate the procedure by computing the piezoelectric and nonlinear dielectric susceptibility tensors of III-V semiconductors.

cond-mat.mtrl-sci↗
arXiv2001

Maximally-localized Wannier functions for entangled energy bands

We present a method for obtaining well-localized Wannier-like functions (WFs) for energy bands that are attached to or mixed with other bands. The present scheme removes the limitation of the usual maximally-localized WFs method (N. Marzari and D. Vanderbilt, Phys. Rev. B 56, 12847 (1997)) that the bands of interest should form an isolated group, separated by gaps from higher and lower bands everywhere in the Brillouin zone. An energy window encompassing N bands of interest is specified by the user, and the algorithm then proceeds to disentangle these from the remaining bands inside the window by filtering out an optimally connected N-dimensional subspace. This is achieved by minimizing a functional that measures the subspace dispersion across the Brillouin zone. The maximally-localized WFs for the optimal subspace are then obtained via the algorithm of Marzari and Vanderbilt. The method, which functions as a postprocessing step using the output of conventional electronic-structure codes, is applied to the s and d bands of copper, and to the valence and low-lying conduction bands of silicon. For the low-lying nearly-free-electron bands of copper we find WFs which are centered at the tetrahedral interstitial sites, suggesting an alternative tight-binding parametrization.

cond-mat.mtrl-sci↗
arXiv2000

Wannier-function description of the electronic polarization and infrared absorption of high-pressure hydrogen

We have constructed maximally-localized Wannier functions for prototype structures of solid molecular hydrogen under pressure, starting from LDA and tight-binding Bloch wave functions. Each occupied Wannier function can be associated with two paired protons, defining a ``Wannier molecule''. The sum of the dipole moments of these ``molecules'' always gives the correct macroscopic polarization, even under strong compression, when the overlap between nearby Wannier functions becomes significant. We find that at megabar pressures the contributions to the dipoles arising from the overlapping tails of the Wannier functions is very large. The strong vibron infrared absorption experimentally observed in phase III, above ~ 150 GPa, is analyzed in terms of the vibron-induced fluctuations of the Wannier dipoles. We decompose these fluctuations into ``static'' and ``dynamical'' contributions, and find that at such high densities the latter term, which increases much more steeply with pressure, is dominant.

cond-mat.mtrl-sci↗
arXiv2000

Polarization and localization in insulators: generating function approach

We develop the theory and practical expressions for the full quantum-mechanical distribution of the intrinsic macroscopic polarization of an insulator in terms of the ground state wavefunction. The central quantity is a cumulant generating function which yields, upon successive differentiation, all the cumulants and moments of the probability distribution of the center of mass X/N of the electrons, defined appropriately to remain valid for extended systems obeying twisted boundary conditions. The first moment is the average polarization, where we recover the well-known Berry phase expression. The second cumulant gives the mean-square fluctuation of the polarization, which defines an electronic localization length xi_i along each direction i. It follows from the fluctuation-dissipation theorem that in the thermodynamic limit xi_i diverges for metals and is a finite, measurable quantity for insulators. It is possible to define for insulators maximally-localized ``many-body Wannier functions'', which for large N become localized in disconnected regions of the high-dimensional configuration space, establishing a direct connection with Kohn's theory of the insulating state. Interestingly, the expression for xi_i^2, which involves the second derivative of the wavefunction with respect to the boundary conditions, is directly analogous to Kohn's formula for the ``Drude weight'' as the second derivative of the energy.

cond-mat↗
arXiv1998

Polarization and Strong Infra-Red Activity in Compressed Solid Hydrogen

Under a pressure of ~150 GPa solid molecular hydrogen undergoes a phase transition accompanied by a dramatic rise in infra-red absorption in the vibron frequency range. We use the Berry's phase approach to calculate the electric polarization in several candidate structures finding large, anisotropic dynamic charges and strongly IR-active vibron modes. The polarization is shown to be greatly affected by the overlap between the molecules in the crystal, so that the commonly used Clausius-Mossotti description in terms of polarizable, non-overlapping molecular charge densities is inadequate already at low pressures and even more so for the compressed solid.

cond-mat↗
arXiv1997

Metric tensor as the dynamical variable for variable cell-shape molecular dynamics

We propose a new variable cell-shape molecular dynamics algorithm where the dynamical variables associated with the cell are the six independent dot products between the vectors defining the cell instead of the nine cartesian components of those vectors. Our choice of the metric tensor as the dynamical variable automatically eliminates the cell orientation from the dynamics. Furthermore, choosing for the cell kinetic energy a simple scalar that is quadratic in the time derivatives of the metric tensor, makes the dynamics invariant with respect to the choice of the simulation cell edges. Choosing the densitary character of that scalar allows us to have a dynamics that obeys the virial theorem. We derive the equations of motion for the two conditions of constant external pressure and constant thermodynamic tension. We also show that using the metric as variable is convenient for structural optimization under those two conditions. We use simulations for Ar with Lennard-Jones parameters and for Si with forces and stresses calculated from first-principles of density functional theory to illustrate the applications of the method.

cond-mat↗