High Luminescence in Small Si/SiO2 Nanocrystals: A Theoretical Study

TL;DR

This theoretical study investigates the factors influencing photoluminescence in Si/SiO2 nanocrystals, highlighting the roles of size, surface termination, and interface chemistry in optimizing optical emission.

Contribution

It provides a theoretical analysis of radiative recombination rates in various Si/SiO2 nanocrystals, revealing new insights into how interface chemistry affects luminescence efficiency.

Findings

Recombination rates follow quantum confinement for hydrogenated nanocrystals.

Interface oxygen content significantly impacts recombination rates.

High crystallinity and small size enhance optical emission.

Abstract

In recent years many experiments have demonstrated the possibility to achieve efficient photoluminescence from Si/SiO2 nanocrystals. While it is widely known that only a minor portions of the nanocrystals in the samples contribute to the observed photoluminescence, the high complexity of the Si/SiO2 interface and the dramatic sensitivity to the fabrication conditions make the identification of the most active structures at the experimental level not a trivial task. Focusing on this aspect we have addressed the problem theoretically, by calculating the radiative recombination rates for different classes of Si-nanocrystals in the diameter range of 0.2-1.5 nm, in order to identify the best conditions for optical emission. We show that the recombination rates of hydrogenated nanocrystals follow the quantum confinement feature in which the nanocrystal diameter is the principal quantity in determining the system response. Interestingly, a completely different behavior emerges from the OH-terminated or SiO2-embedded nanocrystals, where the number of oxygens at the interface seems intimately connected to the recombination rates, resulting the most important quantity for the characterization of the optical yield in such systems. Besides, additional conditions for the achievement of high rates are constituted by a high crystallinity of the nanocrystals and by high confinement energies (small diameters).