Defects and strain enhancements of second-harmonic generation in Si/Ge superlattices

International audienceStarting from experimental findings and interface growth problems in Si/Ge superlattices, we have investigated through ab initio methods the concurrent and competitive behavior of strain and defects in the second-harmonic generation process. Interpreting the second-harmonic intensities as a function of the different nature and percentage of defects together with the strain induced at the interface between Si and Ge, we found a way to tune and enhance the second-harmonic generation response of these systems. (C) 2014 AIP Publishing LLC

Resonant optical control of the structural distortions that drive ultrafast demagnetization in Cr2_2O3_3

We study how the color and polarization of ultrashort pulses of visible light can be used to control the demagnetization processes of the antiferromagnetic insulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation (SHG) to probe how changes in the magnetic and structural state evolve in time. We show that, varying the pump photon-energy to excite either localized transitions within the Cr or charge transfer states, leads to markedly different dynamics. Through a full polarization analysis of the SHG signal, symmetry considerations and density functional theory calculations, we show that, in the non-equilibrium state, SHG is sensitive to {\em both} lattice displacements and changes to the magnetic order, which allows us to conclude that different excited states couple to phonon modes of different symmetries. Furthermore, the spin-scattering rate depends on the induced distortion, enabling us to control the timescale for the demagnetization process. Our results suggest that selective photoexcitation of antiferromagnetic insulators allows fast and efficient manipulation of their magnetic state.Comment: 7 pages, 5 figure

Ab Initio Second-Order Nonlinear Optics in Solids: Second-Harmonic Generation Spectroscopy from Time-Dependent Density-Functional Theory

We present in detail the formulation of the ab initio theory we have developed for the calculation of the macroscopic second-order susceptibility $\chi^{(2)}$. We find a general expression for $\chi^{(2)}$ valid for any fields, containing the ab initio relation between the \textit{microscopic} and \textit{macroscopic} formulation of the second-order responses. We consider the long wavelength limit and we develop our theory in the Time-Dependent Density-Functional Theory framework. This allows us to include straightforwardly many-body effects such as crystal local-field and excitonic effects. We compute the Second-Harmonic Generation spectra for the cubic semiconductors SiC, AlAs and GaAs and starting from the Independent-Particle Approximation for $\chi^{(2)}$, we include quasiparticle effects via the scissors operator, crystal local-field and excitonic effects. In particular, we consider two different types of kernels: the ALDA and the "long-range" kernel. We find good agreement with other theoretical calculations and experiments presented in literature, showing the importance of very accurate description of the many-body interactions

Dynamical ionization ignition of clusters in intense and short laser pulses

The electron dynamics of rare gas clusters in laser fields is investigated quantum mechanically by means of time-dependent density functional theory. The mechanism of early inner and outer ionization is revealed. The formation of an electron wave packet inside the cluster shortly after the first removal of a small amount of electron density is observed. By collisions with the cluster boundary the wave packet oscillation is driven into resonance with the laser field, hence leading to higher absorption of laser energy. Inner ionization is increased because the electric field of the bouncing electron wave packet adds up constructively to the laser field. The fastest electrons in the wave packet escape from the cluster as a whole so that outer ionization is increased as well.Comment: 8 pages, revtex4, PDF-file with high resolution figures is available from http://mitarbeiter.mbi-berlin.de/bauer/publist.html, publication no. 24. Accepted for publication in Phys. Rev.

Linear electro-optic effect in semiconductors: Ab initio description of the electronic contribution

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Long-range corrected exchange-correlation kernels to describe excitons in second-harmonic generation

International audienceWe investigate the role of excitons in second-harmonic generation (SHG) through the long-range corrected (LRC) exchange-correlation kernels: empirical LRC, Bootstrap, and jellium-with-a-gap model. We calculate the macroscopic second-order frequency-dependent susceptibility χ(2). We also present the frequency-dependent macroscopic dielectric function ϵM which is a fundamental quantity in the theoretical derivation of χ(2). We assess the role of the long-range kernels in describing excitons in materials with different symmetry types: cubic zincblende, hexagonal wurtzite, and tetragonal symmetry. Our studies indicate that excitons play an important role in χ(2) bringing a strong enhancement of the SHG signal. Moreover, we found that the SHG enhancement follows a simple trend determined by the magnitude of the long-range corrected α-parameter. This trend is material dependent

Ab initio calculation of many-body effects on the second-harmonic generation spectra of hexagonal SiC polytypes

International audienceWe investigate the influence of crystal local fields and excitonic effects on the spectrum of the second harmonic generation of three polytypes of silicon carbide by using time-dependent density-functional theory including many-body effects, namely, quasiparticle corrections through the scissors operator, crystal local field effects, and excitonic interaction. The relation between the scalar density response and the components of the rank 3 tensor d(2) is established by calculating the response along different polarization directions. We find that local-field effects, although necessary for a rigorous description in the theory, yield only small contributions to the spectra, whereas excitonic effects have a strong influence on the second harmonic generation. We compare static values of the second harmonic coefficients to recent measurements and obtain very good agreement

Electron energy loss spectroscopy of thin slabs with supercell calculations

International audienceElectron energy loss spectroscopy in the low loss regime is widely used to access to the screening of the Coulomb potential as a function of the momentum transfer. This screening is strongly reduced for low dimensional materials and this spectroscopy is a technique of choice to study the resulting quantum connement. Time-dependent density functional theory within an ab initio formalism, is particularly suited to simulate angular resolved electron energy loss spectra, taking benet from the reciprocal space description. For an isolated object, the standard procedure based on the supercell approach dramatically fails for the out-of-plane optical response of the surface and we have proposed a new scheme called Selected-G, 1 leading to a slab potential. In this paper, we show that the standard procedure also aects the in-plane components of the EEL spectra. Applying the Selected-G procedure, we show that the full expression of the slab potential is crucial to describe slabs of nite thickness. We compare our formalism to other cuto procedures, and show that if they provide spectra with the correct spectral weight, allowing the good description of plasmon dispersion, the amplitude of the peaks depends on the choice of the supercell. Our results, which provide spectra independent of vacuum, will have a strong impact on the calculation of properties such as quasiparticle corrections