[Calculs ab-initio de la luminescence et des propriétés de gain optique dans des nanostructures de silicium]
Nous avons effectué des calculs en théorie de la fonctionnelle de la densité et en théorie des perturbations à plusieurs corps dans le but d'étudier les propriétés optiques de nanocristaux de silicium dans plusieurs conditions de passivations de surface, et dans des configurations soit d'état fondamental soit d'état excité. En partant d'agrégats hydrogénés, nous avons considéré différentes géométries de liaison Si/O à l'interface. Nos résultats indiquent qu'il faut prendre en compte non seulement les effets de confinement quantique mais aussi la chimie de l'interface, pour bien comprendre les propriétés physiques de ces systèmes. En particulier nous montrons que seule la présence d'une liaison « bridge » Si–O–Si à la surface permet d'induire un pic excitonique dans le spectre d'émission, avec un déplacement vers le rouge par rapport au seuil d'absorption, permettant d'expliquer le déplacement de Stokes observé, et la PL dans le proche visible observée expérimentalement dans Si-nc. Pour les cristaux de silicium dans une matrice de SiO2, les propriétés optiques sont discutées en détail. L'interaction forte entre le nanocristal et l'environnement, et le rôle actif de la région d'interface entre les deux, sont mis en évidence, en très bon accord avec les résultats expérimentaux. Pour chacun des systèmes considérés, des calculs de gain optique ont été effectués, donnant des pistes concernant les caractéristiques nécessaires pour optimiser la performance de gain optique des Si-nc.
Density-functional and many body perturbation theory calculations have been carried out in order to study the optical properties both in the ground and excited state configurations, of silicon nanocrystals in different conditions of surface passivation. Starting from hydrogenated clusters, we have considered different Si/O bonding geometries at the interface. We provide strong evidence that not only the quantum confinement effect but also the chemistry at the interface has to be taken into account in order to understand the physical properties of these systems. In particular, we show that only the presence of a surface Si–O–Si bridge bond induces an excitonic peak in the emission-related spectra, redshifted with respect to the absorption onset, able to provide an explanation for both the observed Stokes shift and the near-visible PL experimentally observed in Si-nc. For the silicon nanocrystals embedded in a SiO2 matrix, the optical properties are discussed in detail. The strong interplay between the nanocrystal and the surrounding host environment and the active role of the interface region between them is pointed out, in very good agreement with the experimental results. For each system considered, optical gain calculations have been carried out giving some insights on the system characteristics necessary to optimize the gain performance of Si-nc.
Mots-clés : Nanocristaux, Silicium, Propriétés optiques, Gain
Elena Degoli 1 ; Roberto Guerra 2 ; Federico Iori 2 ; Rita Magri 2 ; Ivan Marri 2 ; Olivia Pulci 3 ; Olmes Bisi 1 ; Stefano Ossicini 1
@article{CRPHYS_2009__10_6_575_0,
author = {Elena Degoli and Roberto Guerra and Federico Iori and Rita Magri and Ivan Marri and Olivia Pulci and Olmes Bisi and Stefano Ossicini},
title = {Ab-initio calculations of luminescence and optical gain properties in silicon nanostructures},
journal = {Comptes Rendus. Physique},
pages = {575--586},
publisher = {Elsevier},
volume = {10},
number = {6},
year = {2009},
doi = {10.1016/j.crhy.2008.09.003},
language = {en},
}
TY - JOUR AU - Elena Degoli AU - Roberto Guerra AU - Federico Iori AU - Rita Magri AU - Ivan Marri AU - Olivia Pulci AU - Olmes Bisi AU - Stefano Ossicini TI - Ab-initio calculations of luminescence and optical gain properties in silicon nanostructures JO - Comptes Rendus. Physique PY - 2009 SP - 575 EP - 586 VL - 10 IS - 6 PB - Elsevier DO - 10.1016/j.crhy.2008.09.003 LA - en ID - CRPHYS_2009__10_6_575_0 ER -
%0 Journal Article %A Elena Degoli %A Roberto Guerra %A Federico Iori %A Rita Magri %A Ivan Marri %A Olivia Pulci %A Olmes Bisi %A Stefano Ossicini %T Ab-initio calculations of luminescence and optical gain properties in silicon nanostructures %J Comptes Rendus. Physique %D 2009 %P 575-586 %V 10 %N 6 %I Elsevier %R 10.1016/j.crhy.2008.09.003 %G en %F CRPHYS_2009__10_6_575_0
Elena Degoli; Roberto Guerra; Federico Iori; Rita Magri; Ivan Marri; Olivia Pulci; Olmes Bisi; Stefano Ossicini. Ab-initio calculations of luminescence and optical gain properties in silicon nanostructures. Comptes Rendus. Physique, Theoretical spectroscopy, Volume 10 (2009) no. 6, pp. 575-586. doi : 10.1016/j.crhy.2008.09.003. https://comptes-rendus.academie-sciences.fr/physique/articles/10.1016/j.crhy.2008.09.003/
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