Enhanced Radiative Transition in Si_nGe_m Nanoclusters

TL;DR

This study uses ab-initio simulations to analyze SiGe nanoclusters, revealing that hydrogen passivation removes defect states and significantly enhances radiative transitions, especially around Ge atoms, leading to increased photoluminescence.

Contribution

It demonstrates that hydrogen passivation improves the optical properties of SiGe nanoclusters by removing defect states and boosting radiative transition rates, a novel insight for nanocluster engineering.

Findings

Hydrogen passivation removes defect states and opens the energy gap.

Radiative transition rates are increased by one to two orders of magnitude.

Enhanced overlap of HOMO and LUMO wavefunctions on Ge atoms explains emission increase.

Abstract

Using an ab-initio molecular dynamics scheme (the Fireball scheme), we determined the equilibrium structure of intermediate size Si_nGe_m (n+m=71) nanoclusters with/without hydrogen passivation on the surface. Due to the strong surface distortion, defect states are found to permeate the energy gap of Si_nGe_m clusters. However, the defect states are removed by adding H atoms on the surface of Si_nGe_m clusters, and the gap opens up to a few eV, indicating a blueshift for photoluminescence. It is also found that the radiative transition between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) states is enhanced by one to two orders of magnitude for Si_nGe_m nanoclusters with respect to the corresponding pure Si clusters. This significant increase of the emission probability is attributed to the strong overlap of HOMO and LUMO wavefunctions that are centered mostly on the Ge atoms.