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First principles Second-Harmonic Generation in quantum confined silicon-based systems

Matteo Bertocchi 1
1 ST - Spectroscopie théorique
LSI - Laboratoire des Solides Irradiés
Abstract : In this thesis I have dealt with the ab initio description of the second-harmonic generation (SHG) process, a nonlinear optical property of materials, focusing in particular on quantum confined, silicon-based systems. In the last decades, the accuracy and possibilities of ab initio studies have demonstrated a great relevance in both the interpretation and prediction of the materials properties. It is then mandatory to improve the knowledge of the nonlinear optical processes as well as the SHG first-principle description. Nowadays, due to nontrivial difficulties, nonlinear optics has not yet reached the accuracy and development of linear phenomena. In particular, the state of the art of ab initio SHG calculations is represented by the inclusion of many-body effects as crystal local fields (LF) and electron-hole interaction, but today, the mostly used approach is the independent particle approximation (IPA), the only one able to approach calculations of complex structures such as surfaces and interfaces. Whereas IPA can be a good approximation for bulk systems, in discontinuous materials other effects may be predominant. Hence their description is of great relevance although the lack of studies. My thesis tries to give a first analysis of the SHG process in more complex systems as the interfaces and the Si-confined systems, inferring new insights on the physical mechanism and its link with the nature of the system. I use an efficient formalism based on the Time Dependent Density Functional Theory (TDDFT) where many-body effects are included via an appropriate choice of the TDDFT kernels. Both the formalism and the code have been developed during the thesis work permitting the study complex materials. The research has been focused on the Si(111)/CaF2 (T4 B-type) interface case study. Convergence studies show the importance of the semiconductor material with respect to the insulator. The response is characteristic of a deep region beyond the Si interface whereas the CaF2 converges soon after the first interface layers. Moreover, the signal demonstrates to be sensitive to the electronic-states modifications that are induced far below the interface, and not to the Si ionic structure that recovers soon the bulk configuration. A normalization procedure to compare with the experiment has been proposed. The SHG spectra have been calculated in the IPA, introducing LF and excitonic interactions. New behaviors have been observed with respect to the SHG processes on strained silicon, GaAs or SiC showing in particular the importance of crystal local-field effects with respect to both the IPA and the excitons. Whereas IPA can describe the position of the SHG main peaks and the excitonic effects slightly modify the total intensity, only LF are able to correctly reproduce the spectral shape and the relative intensities of the peaks. This underlines how SHG and the different involved effects depends on the nature of the materials. New methods of analysis of the response have been proposed; actually, the direct link between the peaks position and the transition energies is lost in SHG calculations (i.e. the signal comes from a second order Dyson equation where linear and nonlinear response functions at different frequencies are mixed together). Furthermore, the complexity of the system allowed me to extend the study to a large variety of materials as the multilayers and the silicon confined slabs. The results show a good agreement with the experiment confirming the proposed T4 B-type interface structure. This underlines the accuracy of the formalism, the possibility of improving our knowledge on these complex materials going beyond the standard approaches, and confirms the possibility of SHG ab-initio simulations to be employed as a predictive technique, supporting and guiding experiments and technological developments. Preliminary results on Si/Ge superlattice are presented.
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Submitted on : Thursday, March 7, 2013 - 12:23:44 PM
Last modification on : Monday, February 10, 2020 - 6:14:04 PM
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Matteo Bertocchi. First principles Second-Harmonic Generation in quantum confined silicon-based systems. Materials Science [cond-mat.mtrl-sci]. Ecole Polytechnique X, 2013. English. ⟨pastel-00796933⟩

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